TWI240957B - Manufacturing method for crystal film using laser and the crystal film - Google Patents

Manufacturing method for crystal film using laser and the crystal film Download PDF

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Publication number
TWI240957B
TWI240957B TW092129598A TW92129598A TWI240957B TW I240957 B TWI240957 B TW I240957B TW 092129598 A TW092129598 A TW 092129598A TW 92129598 A TW92129598 A TW 92129598A TW I240957 B TWI240957 B TW I240957B
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TW
Taiwan
Prior art keywords
laser beam
band
crystal grains
pulsed laser
region
Prior art date
Application number
TW092129598A
Other languages
Chinese (zh)
Other versions
TW200416835A (en
Inventor
Toshio Kudo
Kouji Seike
Kazunori Yamazaki
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Sumitomo Heavy Industries
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Application filed by Sumitomo Heavy Industries filed Critical Sumitomo Heavy Industries
Publication of TW200416835A publication Critical patent/TW200416835A/en
Application granted granted Critical
Publication of TWI240957B publication Critical patent/TWI240957B/en

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
    • H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
    • H01L21/02104—Forming layers
    • H01L21/02365—Forming inorganic semiconducting materials on a substrate
    • H01L21/02656—Special treatments
    • H01L21/02664—Aftertreatments
    • H01L21/02667—Crystallisation or recrystallisation of non-monocrystalline semiconductor materials, e.g. regrowth
    • H01L21/02675—Crystallisation or recrystallisation of non-monocrystalline semiconductor materials, e.g. regrowth using laser beams
    • H01L21/02686—Pulsed laser beam
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
    • H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
    • H01L21/04—Manufacture or treatment of semiconductor devices or of parts thereof the devices having potential barriers, e.g. a PN junction, depletion layer or carrier concentration layer
    • H01L21/18—Manufacture or treatment of semiconductor devices or of parts thereof the devices having potential barriers, e.g. a PN junction, depletion layer or carrier concentration layer the devices having semiconductor bodies comprising elements of Group IV of the Periodic Table or AIIIBV compounds with or without impurities, e.g. doping materials
    • H01L21/20—Deposition of semiconductor materials on a substrate, e.g. epitaxial growth solid phase epitaxy
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
    • H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
    • H01L21/02104—Forming layers
    • H01L21/02365—Forming inorganic semiconducting materials on a substrate
    • H01L21/02367—Substrates
    • H01L21/0237—Materials
    • H01L21/02422—Non-crystalline insulating materials, e.g. glass, polymers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
    • H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
    • H01L21/02104—Forming layers
    • H01L21/02365—Forming inorganic semiconducting materials on a substrate
    • H01L21/02436—Intermediate layers between substrates and deposited layers
    • H01L21/02439—Materials
    • H01L21/02441—Group 14 semiconducting materials
    • H01L21/0245—Silicon, silicon germanium, germanium
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
    • H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
    • H01L21/02104—Forming layers
    • H01L21/02365—Forming inorganic semiconducting materials on a substrate
    • H01L21/02436—Intermediate layers between substrates and deposited layers
    • H01L21/02439—Materials
    • H01L21/02488—Insulating materials
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
    • H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
    • H01L21/02104—Forming layers
    • H01L21/02365—Forming inorganic semiconducting materials on a substrate
    • H01L21/02656—Special treatments
    • H01L21/02664—Aftertreatments
    • H01L21/02667—Crystallisation or recrystallisation of non-monocrystalline semiconductor materials, e.g. regrowth
    • H01L21/02675—Crystallisation or recrystallisation of non-monocrystalline semiconductor materials, e.g. regrowth using laser beams
    • H01L21/02678—Beam shaping, e.g. using a mask
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
    • H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
    • H01L21/02104—Forming layers
    • H01L21/02365—Forming inorganic semiconducting materials on a substrate
    • H01L21/02656—Special treatments
    • H01L21/02664—Aftertreatments
    • H01L21/02667—Crystallisation or recrystallisation of non-monocrystalline semiconductor materials, e.g. regrowth
    • H01L21/02691—Scanning of a beam
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
    • H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
    • H01L21/04—Manufacture or treatment of semiconductor devices or of parts thereof the devices having potential barriers, e.g. a PN junction, depletion layer or carrier concentration layer
    • H01L21/18—Manufacture or treatment of semiconductor devices or of parts thereof the devices having potential barriers, e.g. a PN junction, depletion layer or carrier concentration layer the devices having semiconductor bodies comprising elements of Group IV of the Periodic Table or AIIIBV compounds with or without impurities, e.g. doping materials
    • H01L21/26—Bombardment with radiation
    • H01L21/263—Bombardment with radiation with high-energy radiation
    • H01L21/268—Bombardment with radiation with high-energy radiation using electromagnetic radiation, e.g. laser radiation

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  • Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • Power Engineering (AREA)
  • General Physics & Mathematics (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Computer Hardware Design (AREA)
  • Manufacturing & Machinery (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • Optics & Photonics (AREA)
  • Chemical & Material Sciences (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Crystallography & Structural Chemistry (AREA)
  • Toxicology (AREA)
  • Health & Medical Sciences (AREA)
  • Electromagnetism (AREA)
  • Materials Engineering (AREA)
  • Recrystallisation Techniques (AREA)

Abstract

The present invention is to form the working object as thin film composed by amorphous material. A pulsating laser beam with long beam profile in one direction on the surface of the thin film is irradiating into the thin film to melt the thin film, which is then solidified and crystals, connected along the long axis direction in the area between the extended edge along the long axis direction of the beam irradiation area and the center line from the edge and in the first belt area along the long axis direction from the center line with a certain distance, are generated.

Description

1240957 (1) 玖、發明說明 【發明所屬之技術領域】 本發明係有關結晶膜之製造方法及結晶膜，特別是有 關在非結晶膜使雷射光束射入而結晶化之結晶膜之製造方 法及被製造之結晶膜。 結晶膜係能使用於低溫型多結晶τ F T液晶顯示器、 太陽電池脈衝、薄型液晶顯示器、有機E L顯示器等。 【先前技術】 使準分子雷射射入非結晶矽薄膜後反覆進行溶融以及 固化’且在橫方向（薄膜之面內方向）使結晶生長的逐次 的檢方向生長（SLS· Sequential Lateral Solidification) 技術係習知之技術。以下，就從前之SLS技術加以說明 〇 使脈衝雷射光束之剖面長尺寸化後，例如可通過寬幅 3〜30/im、長度左右的狹縫。使通過狹縫之脈衝 雷射光束’通過使狹縫成像於非結晶矽薄膜表面的成像光 學系，而射入非結晶矽膜。該成像光學系的倍率爲例如1 / 3。此時’在非結晶矽膜之表面形成的被雷射光束照射 區域的寬幅約爲1〜1 0 # m、長度約爲3 3 # m。被照射區 域的寬幅方向的光束強度分佈形成近似矩形。 雷射光束射入非結晶矽膜時，非結晶矽會溶融。因爲 溶融之區域的邊緣附近部分的冷卻速度會比內部的冷卻速 度快，所以會從邊緣附近部分開始固化。已固化部分成爲 -5- 1240957 (2) 晶核，且從該晶核向溶融部分之內側使結晶生長。因爲結 晶生長是從被照射區域之長的一方的2個邊緣開始，所以 在被照射區域之寬幅方向的幾乎中央處會形成從兩側生長 而來的結晶粒之粒界。 使脈衝雷射光束之被照射區域朝該寬幅方向僅移動約 該寬幅的5 0 %，使脈衝雷射光束第2次射入。在脈衝雷 射光束第1次照射時之被照射區域的幾乎中央處被形成的 粒界之單側的區域會再溶融。未再溶融之區域的結晶粒會 成爲種晶，且於再溶融之區域使結晶生長。 藉由使脈衝雷射光束之被照射區域移動，同時反覆進 行雷射照射，能使結晶朝被照射區域之移動方向生長。 在以下之專利文獻1〜3所揭示之技術爲：採用Nd : YAG雷射之第2諧波，將光束剖面整形成線狀，照射到 非結晶矽層，且朝橫方向使結晶生長。此外，在專利文獻 4以及5所揭示之技術爲：採用準分子雷射，通過被圖案 化之遮罩照射到非結晶矽層，且朝橫方向使結晶生長。 (專利文獻1 )日本專利特開2000-26073 1號公報 (專利文獻2 )日本專利特開2000-2 86 1 95號公報 (專利文獻3 )日本專利特開2000-2 8 62 1 1號公報 (專利文獻4 )日本專利特開2000-50524 1號公報 (專利文獻5 )日本專利特開2000_274〇88號公報 技術期待能形成更大之結晶粒。本發明之目的係提供 一種在橫方向使結晶生長的新技術。 1240957 (3) 【發明內容】 造方法 晶質材 述薄膜 朝該薄 長軸方 以及該 第1帶 程。 製造方 結晶質 前述薄 束朝該 ，在以 被隔開 被劃定 晶粒， 所產生 晶粒相 雷射光 帶狀區 // m以 依照本發明之一觀點，提供一種多結晶膜之製 ’其特徵爲具有：（a )準備在表面上形成由非結 料構成之薄膜之加工對象物的工程，及（b )在前 之表面使在一方向具有長光束剖面之脈衝雷射光束 膜射入，使該薄膜溶融後固化，在光束射入區域的 向延伸之邊緣與中心線之間的區域之中，自該邊緣 中心線起僅被隔開某段距離的延伸於該長軸方向之 狀區域內》產生在該長軸方向上連接之結晶粒之工 依照本發明之另一觀點，提供一種多結晶膜之 法，其特徵爲具有·· （i)準備在表面上形成由非 材料構成之薄膜之加工對象物的工程，及（j)在 膜之表面使在一方向具有長光束剖面之脈衝雷射光 薄膜射入，使該薄膜溶融後固化使多結晶化之工程 自光束射入區域之長軸方向所延伸之邊緣向內側僅 某段距離的假想線，與以該光束射入區域之中心線 之第1帶狀區域內，產生在該長軸方向上連接之結 而使前述中心線之一方之側的前述第1帶狀區域內 之結晶粒，與另一方之第1帶狀區域內所產生之結 互接觸的條件下使脈衝雷射光束射入之工程；脈衝 束之脈衝能量密度的短軸方向的梯度，於前述第1 域的長軸方向所延伸的外側緣，爲280mJ/ cm2/ 下。 依照本發明之另一觀點，提供一種多結晶膜之製造方 (4) 1240957 法，其特徵爲具有：（p )準備在表面上形成由非結晶質 材料構成之薄膜之加工對象物的工程，及（q )在前述薄 膜之表面使在一方向具有長光束剖面之脈衝雷射光束朝該 薄膜射入，使該薄膜溶融後固化使多結晶化之工程，其中 脈衝雷射光束之射入工程之光束密度分佈（profile)方面 ’即脈衝雷射光束之脈衝能量密度之短軸方向的梯度，於 已溶融區域之邊緣爲280mJ / cm2/ // m以下。 藉由在上述條件下照射脈衝雷射光束，能形成大的結 晶粒。 【實施方式】 第1圖係顯示本發明之實施例中被使用之雷射退火裝 置的槪略圖。雷射退火裝置之構成包含處理室4〇、搬送 室82、搬出入室83、84、雷射光源71、均質器72、CCD 攝影器88以及錄影監視器89。在處理室40安裝包含伸 縮軟管67、結合構件63、65、線性導引機構64以及線性 馬達6 6等之滑動機構6 〇。滑動機構6 〇能使被配置在處 理室40內之平臺44並進移動。 處理室40與搬送室82中介著閘閥85而被結合，搬 送室82與搬出入室83、以及搬送室82與搬出入室84則 分別中介著閘閥86以及87而被結合。在處理室40、搬 出入室83以及84分別安裝真空泵浦91、92以及93，可 將各室之內部排氣成真空。 在搬送室82內收容搬送用機器手臂94。搬送用機器 -8 · 1240957 (5) 手臂94係於處理室40、搬出入室83以及84之各室相互 間移送處理基板。 在處理室40的上面設置雷射光束透過用之石英窗38 。又，除石英外，採用 BK7等可視光學玻璃取代亦可。 從雷射光源7 1被輸出之脈衝雷射光束通過哀減器7 6後射 入均質器72。均質器72會將雷射光束之剖面形狀作成細 長形狀，而且將關於該長軸方向之強度作成一致。通過均 質器72之雷射光束係透過對應於光束之剖面形狀的細長 石英窗38，射入被保持在處理室40內之平臺44上的處 理基板。以作成基板之表面與均質器之面一致的方式，調 節均質器72與處理基板之相對位置。 藉由滑動機構60使平臺44並進移動的方向係垂直於 石英窗38之長邊方向的方向。藉此，能對基板表面之廣 泛區域照射雷射光束，且使形成於基板表面上的非結晶質 半導體膜多結晶化。基板表面可利用C C D攝影器8 8被攝 影，而以錄影監視器8 9觀察處理中的基板表面。 第2 A圖係加工對象物1的剖面圖，以及例示在加工 對象物1表面之有關雷射光束之短軸方向的脈衝能量密度 之分佈。加工對象物1係具有由厚度0.7mm之玻璃基板2 、覆蓋該表面之厚度1 OOnm的氧化矽膜3，以及被形成於 該表面上之厚度50nm的非結晶矽膜4所形成的3層構造 。氧化矽膜3係以例如化學氣相成長（CVD )或者濺鍍而 被形成。非結晶矽膜4則以例如減壓CVD ( LP— CVD ) 或者電漿激發型CVD(PE — CVD)而被形成。 -9- 1240957 (6) 有關光束剖面之短軸方向的脈衝能量密度之分佈5可 以近似於高斯分佈。使非結晶矽完全地溶融之閾値Eth以 上的脈衝能量密度之雷射光束射入之區域6內的非結晶矽 膜4完全地溶融。在此，「完全地」係意味矽膜所有厚度 皆溶融。 在比該區域更外側之，脈衝能量密度從閩値Eth至 Ec之間的區域1 2，矽膜則部分地溶融。在此，「部分地 」係意味砂膜之一部分溶融，亦殘存有維持非結晶狀態而 未溶融的部分。比脈衝能量密度成爲Ec之位置更外側的 區域9的非結晶矽膜4並未溶融。在溶融之矽固化時，形 成矽的結晶粒。 本專利發明者發現：在脈衝能量密度成爲閾値Eth之 位置的附近的帶狀區域7內，會形成比較大的結晶粒，而 在比該區域更內側之區域8內，會形成小的微結晶粒，在 區域1 2內，結晶粒大小介於區域8內之結晶粒與帶狀區 域7內之結晶粒的結晶粒則隨機分佈。在此，「結晶粒大 小」係意味分佈於該區域內的結晶粒之平均大小。 第2B圖係顯示被脈衝雷射光束照射之區域的模式的 平面圖。第2B圖之縱方向爲對應於光束射入區域之長軸 方向。在光束射入區域之長軸方向所延伸之邊緣10與中 心線〗1之間，被配置在長軸方向延伸之帶狀區域7。帶 狀區域7係從光束射入區域之邊緣1 0隔著某段間隔被配 置。在帶狀區域7內形成連接在長軸方向的多數之結晶粒 13° •10- 1240957 (7) 有關脈衝雷射光束之短軸方向的強度分佈係近似於高 斯分佈。將短軸方向之強度分佈的半値幅稱作光束寬幅。 實際上，在加工對象物表面之相當於光束寬幅的區域之兩 側，亦照射高斯分佈之裙襬部之部分的光束成分。光束射 入區域之邊緣1 0，例如可以定義爲脈衝能量密度成爲最 大値之1 0 %的部分。 第3圖係描繪被多結晶化之矽膜的掃瞄型電子顯微鏡 攝影（SEM攝影）。射入之脈衝雷射光束係2倍於Nd : YLF雷射的諧波（波長52 7nm或者5 24nm )，脈衝寬幅 係100ns。加工對象物表面之光束剖面之長軸方向的長度 係5mm，光束寬幅爲0.2mm。 在加工對象物表面使脈衝能量密度爲 5 00m cm2的 2道脈衝雷射光束同時地照射於同一處。因此，實效上的 脈衝能量密度成爲1】/ cm2。又，脈衝能量密度的計算係 根據將脈衝能量除以加工對象物表面的光束剖面之面積。 在帶狀區域7內形成比較大的結晶粒，且這些結晶粒 會在長軸方向連接。這些結晶粒，短軸方向的長度爲1.5 〜左右，長軸方向的大小爲0.7〜左右。在2 條帶狀區域7之間的區域8形成多數微結晶粒。 此外，在比帶狀區域7再外側之區域1 2內，有結晶 粒大於區域8內之微結晶粒，小於帶狀區域7內之結晶粒 的結晶粒被隨機地配置。藉由顯微鏡觀察，能將這些區域 的邊界當作色差檢測出。 其次，就如第3圖所示之種種大小的結晶粒產生的機 -11 - 1240957 (8) 構予以考察。 第4 A圖係顯示矽結晶之生長速度的溫度依存性，第 4 B圖係顯不結晶生長之核生成率的溫度依存性。第4 a圖 之縱軸係以單位1 m / s」表示生長速度，第4 b圖之縱軸 則以單位「1 / c m3 · s」表示核生成率，兩者之橫軸皆以 單位「K」表示溫度。又，第4 A圖以及第4 B圖的圖形係 得自於1 9 9 9年7月1 4日舉行之日本塑性加工學會模擬統 合系統分科會第2 1回FEM專題講座之資料集第22號第 27〜32頁被刊載之市嶋大路（住友重機械工業株式會社 )的「多結晶體之動的結晶成長過程的微解析」的手法。 如第4 A圖所示，在單結晶矽的融點（；[6 8 3 κ )生長 速度爲〇，且隨溫度下降而生長速度變快。在溫度1 5 00K 附近顯示生長速度爲最大値。所以，溶融的矽的溫度愈低 ，結晶生長速度愈快。又，結晶生長速度亦依存於固相部 分與液相部分之界面的溫度梯度，如溫度梯度陡峻則結晶 生長速度快。 如第4B圖所示，核生成率係從矽的融點起隨溫度降 低而變大，顯示在溫度600K附近爲最大値。 第3圖所示之帶狀區域7被認爲係核生成率低且生長 速度快之適當溫度以及在固液界面之適當溫度梯度的區域 。帶狀區域7與非結晶質區域9之間的區域1 2因溫度低 於帶狀區域7故而核生成率高’且因在固液界面的溫度梯 度緩和所以是生長速度遲緩的區域。該區域中’因爲在生 長成大的結晶之前會產生許多的晶核’所以無法生長成大 -12- 1240957 (9) 的結晶粒。 在微結晶區域8方面，一般認爲係藉由溫度的降低使 晶核爆發性地產生，且晶核生成會比結晶生長速度更具支 配性的區域。當溫度被冷卻至核生成率急速變高之溫度時 ，帶狀區域7內之結晶生長會受新產生之晶核所妨礙，使 結晶生長停止。結晶生長停止之處則相當於帶狀區域7與 微結晶區域8之邊界。 更詳細而言，在區域1 2方面，一般認爲來自溶融之 層與其底層之界面所產生的晶核的結晶生長（異質生長） 爲具支配性，而在微結晶區域8方面，則來自溶融之層的 內部所產生的晶核的結晶生長（同質生長）爲具支配性。 在異質生長所支配之區域與同質生長所支配之區域的邊界 會形成大的結晶粒。 爲形成大的結晶粒，必須將矽的溶融部分作成生長速 度快且核生成率低的適當溫度梯度以及溫度。如第2 A圖 所示之帶狀區域7的位置的溫度梯度陡峻，則被維持在適 當溫度之區域會變狹窄，且不易形成大的結晶粒。爲形成 大的結晶粒，將帶狀區域7附近的脈衝能量密度分佈的梯 度作成和緩較佳。 如脈衝能量密度分佈之梯度過於陡峻，核生成率會提 高。另一方面，如脈衝能量密度分佈之梯度過於和緩，結 晶生長速度則變遲緩。因此一般認爲要形成結晶生長速度 快且核生成率低之適當溫度以及固液界面之溫度梯度，須 在脈衝能量密度分佈之梯度具有未過於陡峻且未過於和緩 -13 - 1240957 (10) 之適當範圍。 其/人’參照第5圖，就脈衝能量密度分佈之 予以說明。 第5 A圖係顯示結晶粒大小與在加工對象物 束寬幅的關係圖。橫軸係以單位「# m」表示光 縱軸以單位「V m」表示結晶粒的大小。結晶粒 算係採用在日本專利特開2 0 0 1 - 2 9 7 9 8 3號公報被 晶成長S平價計畫表。 加工對象物係厚度l〇〇nm之氧化矽膜，以 被形成之厚度5 Onm之非結晶矽膜。針對脈衝雷 波長爲5 2 7nm、脈衝寬幅（半値幅）爲14〇ns， 射入區域之中，在比脈衝能量密度爲峰値之一半 外側有1 W m寬幅，內側有5 // m寬幅之合計6 // 區域進行模擬。這是因爲在成爲峰値之一半的値 示脈衝能量密度分佈之梯度爲幾乎最大，所以在 成大的結晶粒。 有關光束射入區域之短軸方向的強度分佈係 分佈。針對光束剖面之寬幅分別爲5.0 // m、8 · 3又 // m，以及8 3.0 e m之4個場合，以種種峰値強 擬，將獲得最大結晶粒之條件下的結晶粒大小作 束寬幅時的結晶粒大小。針對光束剖面之寬幅赁 、8.3//m、16.7"m，以及 83.0/^m 之場合’各 量密度之最大値在 U〇〇mJ/cm2、1 400 mJ/c mJ/ cm2，以及1 5 00 mJ / cm2的條件時可得到最 較佳形狀 表面之光 束寬幅， 大小的計 揭示的結 及在其上 射光束之 針對光束 的位置再 m寬幅的 的位置顯 該區域形 形成高斯 :m、16.7 度進行模 爲在該光 i 5.0 // m 個脈衝能 η2 、 1500 大之結晶 -14- 1240957 (11)1240957 (1) Description of the invention [Technical field to which the invention belongs] The present invention relates to a method for manufacturing a crystalline film and a crystalline film, and particularly to a method for manufacturing a crystalline film that crystallizes by irradiating a laser beam on an amorphous film And the crystalline film being manufactured. The crystalline film system can be used in low-temperature polycrystalline τ F T liquid crystal displays, solar cell pulses, thin liquid crystal displays, organic EL displays, and the like. [Previous technology] SLS · Sequential Lateral Solidification technology that causes the excimer laser to be melted and solidified after being injected into the amorphous silicon film repeatedly and is grown in the lateral direction (in-plane direction of the film). Department of conventional technology. In the following, the previous SLS technology will be described. After the cross-section of the pulsed laser beam has been dimensioned, it can pass through a slit with a width of 3 to 30 / im and about a length. A pulsed laser beam ′ that passes through the slit passes through the imaging optical system that forms the slit on the surface of the amorphous silicon thin film, and then enters the amorphous silicon film. The magnification of the imaging optical system is, for example, 1/3. At this time, the area irradiated by the laser beam formed on the surface of the amorphous silicon film is about 1 to 10 m in width and about 3 3 m in length. The beam intensity distribution in the broad direction of the irradiated area forms an approximately rectangular shape. When the laser beam enters the amorphous silicon film, the amorphous silicon will melt. Because the area near the edge of the molten zone cools faster than the interior, it will begin to solidify near the edge. The solidified part becomes a -5- 1240957 (2) crystal nucleus, and crystals grow from the crystal nucleus to the inside of the molten part. Since the crystal growth starts from the two edges of the long side of the irradiated area, a grain boundary of crystal grains grown from both sides is formed at almost the center in the width direction of the irradiated area. The irradiated area of the pulsed laser beam is moved toward the wide direction by only about 50% of the width, so that the pulsed laser beam is incident for the second time. The area on one side of the grain boundary formed at almost the center of the irradiated area when the pulsed laser beam is irradiated for the first time is re-melted. Crystal grains in unremelted areas become seed crystals, and crystals grow in remelted areas. By moving the irradiated area of the pulsed laser beam and performing laser irradiation repeatedly, the crystal can be grown in the moving direction of the irradiated area. The techniques disclosed in the following Patent Documents 1 to 3 are: using the second harmonic of Nd: YAG laser, shaping the beam profile into a linear shape, irradiating the amorphous silicon layer, and growing crystals in the lateral direction. In addition, the techniques disclosed in Patent Documents 4 and 5 use an excimer laser to irradiate an amorphous silicon layer through a patterned mask and grow crystals in a lateral direction. (Patent Document 1) Japanese Patent Laid-Open No. 2000-26073 1 (Patent Document 2) Japanese Patent Laid-Open No. 2000-2 86 1 95 (Patent Document 3) Japanese Patent Laid-Open No. 2000-2 8 62 1 (Patent Document 4) Japanese Patent Laid-Open No. 2000-50524 1 (Patent Document 5) Japanese Patent Laid-Open No. 2000-274〇88 The technology is expected to form larger crystal grains. The object of the present invention is to provide a new technique for growing crystals in a lateral direction. 1240957 (3) [Summary of the invention] Manufacturing method Crystalline material The thin film faces the thin long axis and the first band. The above-mentioned thin beam of the crystalline material is directed toward the substrate, and the crystal grains are delimited by the partition, and the resulting laser phase bands of the grain phase // m are provided according to an aspect of the present invention to provide a polycrystalline film system. It is characterized by having: (a) a process for preparing a processing object formed of a non-caking film on the surface, and (b) a pulsed laser beam film having a long beam profile in one direction on the front surface The film is cured after being melted. In the area between the extending edge and the center line of the beam incident area, the film extends only a certain distance from the center line of the edge and extends in the direction of the long axis. According to another aspect of the present invention, a method for producing crystal grains connected in the long axis direction is provided, which is characterized by having: (i) preparing to form a non-material on the surface The process of the object of the formed thin film, and (j) a pulsed laser light film having a long beam profile in one direction is injected on the surface of the film, the film is melted and solidified, and the polycrystalline process is projected from the light beam Regional An imaginary line whose edge extending in the axial direction is only a certain distance inward, and a first band-shaped region with the center line of the region where the light beam enters, a knot connected in the long axis direction is generated to make the centerline A process in which a pulsed laser beam is incident under the condition that the crystal grains in the aforementioned first strip-shaped region on one side and the junction generated in the first strip-shaped region of the other are in contact with each other; the pulse energy density of the pulsed beam The gradient in the minor axis direction of ， is 280 mJ / cm2 / under the outer edge extending in the major axis direction of the first domain. According to another aspect of the present invention, there is provided (4) 1240957 method for manufacturing a polycrystalline film, which is characterized by having: (p) a process of preparing a processing object to form a thin film made of an amorphous material on a surface, And (q) a project in which a pulsed laser beam with a long beam profile in one direction is incident on the surface of the aforementioned film, and the film is melted and solidified to crystallize, wherein the pulsed laser beam is projected In terms of beam density profile, the gradient of the short-axis direction of the pulse energy density of the pulsed laser beam is below 280mJ / cm2 / // m at the edge of the melted area. By irradiating a pulsed laser beam under the above conditions, large junction crystal grains can be formed. [Embodiment] Fig. 1 is a schematic diagram showing a laser annealing apparatus used in an embodiment of the present invention. The structure of the laser annealing apparatus includes a processing chamber 40, a transfer chamber 82, carry-in / out chambers 83 and 84, a laser light source 71, a homogenizer 72, a CCD camera 88, and a video monitor 89. The processing chamber 40 is provided with a sliding mechanism 60 including an expansion and contraction hose 67, coupling members 63, 65, a linear guide mechanism 64, a linear motor 66, and the like. The slide mechanism 60 can move the platform 44 disposed in the processing chamber 40 in parallel. The processing chamber 40 and the transfer chamber 82 are coupled via a gate valve 85, and the transfer chamber 82 and the transfer in / out chamber 83 and the transfer chamber 82 and the transfer in / out chamber 84 are coupled via a gate valve 86 and 87, respectively. Vacuum pumps 91, 92, and 93 are installed in the processing chamber 40 and the loading and unloading chambers 83 and 84, respectively, and the inside of each chamber can be evacuated to a vacuum. A transfer robot arm 94 is housed in the transfer chamber 82. Transfer machine -8 · 1240957 (5) The arm 94 is used to transfer processing substrates to each of the processing chamber 40, and the loading and unloading chambers 83 and 84. A quartz window 38 for laser beam transmission is provided on the upper surface of the processing chamber 40. In addition to quartz, optical glass such as BK7 may be used instead. The pulsed laser beam output from the laser light source 71 passes through the attenuator 76 and enters the homogenizer 72. The homogenizer 72 makes the cross-sectional shape of the laser beam into a thin shape, and makes the intensity in the direction of the long axis uniform. The laser beam passing through the homogenizer 72 passes through an elongated quartz window 38 corresponding to the cross-sectional shape of the beam, and is incident on a processing substrate held on a platform 44 held in the processing chamber 40. The relative position of the homogenizer 72 and the processing substrate is adjusted so that the surface of the substrate to be made coincides with the surface of the homogenizer. The direction in which the platform 44 is moved forward by the slide mechanism 60 is a direction perpendicular to the longitudinal direction of the quartz window 38. Thereby, a wide area of the substrate surface can be irradiated with a laser beam, and the amorphous semiconductor film formed on the substrate surface can be polycrystallized. The surface of the substrate can be photographed with a CC camera 8 8 and the surface of the substrate being processed can be observed with a video monitor 8 9. FIG. 2A is a cross-sectional view of the processing object 1 and the distribution of the pulse energy density in the minor axis direction of the laser beam on the surface of the processing object 1 is illustrated. The object 1 has a three-layer structure formed by a glass substrate 2 having a thickness of 0.7 mm, a silicon oxide film 3 having a thickness of 100 nm covering the surface, and an amorphous silicon film 4 having a thickness of 50 nm formed on the surface. . The silicon oxide film 3 is formed by, for example, chemical vapor deposition (CVD) or sputtering. The amorphous silicon film 4 is formed by, for example, reduced pressure CVD (LP-CVD) or plasma-excited CVD (PE-CVD). -9- 1240957 (6) The distribution of the pulse energy density 5 in the short axis direction of the beam profile can be approximated as a Gaussian distribution. The amorphous silicon film 4 in the region 6 into which the laser beam having a pulse energy density above the threshold 値 Eth that the amorphous silicon is completely melted is completely melted. Here, "completely" means that all thicknesses of the silicon film are melted. Outside the region, the pulse energy density is from the region 12 between Eth to Ec, and the silicon film is partially melted. Here, "partially" means that a part of the sand film is partially melted, and a part that remains in an amorphous state and remains unmelted remains. The amorphous silicon film 4 in the region 9 further outside the position where the pulse energy density becomes Ec is not melted. When the molten silicon solidifies, crystal grains of silicon are formed. The inventor of the present patent has found that relatively large crystal grains are formed in the band-shaped region 7 near the position where the pulse energy density becomes the threshold 値 Eth, and small micro-crystals are formed in the region 8 which is more inner than the region In the region 12, the crystal grains having a crystal grain size between the region 8 and the crystal grains in the band-like region 7 are randomly distributed. Here, the "crystal grain size" means the average size of crystal grains distributed in the area. Figure 2B is a plan view showing the pattern of the area illuminated by the pulsed laser beam. The longitudinal direction in Fig. 2B is the long axis direction corresponding to the light beam incident area. Between the edge 10 extending in the long axis direction of the light beam incident region and the center line 1, a strip-shaped region 7 extending in the long axis direction is arranged. The band-like region 7 is arranged from the edge 10 of the beam-entering region at a certain interval. The majority of crystal grains connected in the long-axis direction are formed in the band-like region 7 13 ° • 10-1240957 (7) The intensity distribution of the short-axis direction of the pulsed laser beam is approximately Gaussian. The half width of the intensity distribution in the short-axis direction is called the beam width. In fact, on both sides of the surface of the object to be processed, the beam component of the skirt portion of the Gaussian distribution is also irradiated on both sides of the region corresponding to the width of the beam. The edge 10 of the incident area of the light beam can be defined, for example, as a portion where the pulse energy density becomes a maximum of 10%. Fig. 3 is a scanning electron microscope photograph (SEM photograph) depicting a polycrystalline silicon film. The incoming pulsed laser beam is 2 times the harmonic of Nd: YLF laser (wavelength 52 7nm or 5 24nm), and the pulse width is 100ns. The length in the long axis direction of the beam profile on the surface of the object to be processed is 5 mm, and the beam width is 0.2 mm. Two pulse laser beams with a pulse energy density of 500 m cm2 were irradiated on the surface of the object at the same place at the same time. Therefore, the effective pulse energy density becomes 1] / cm2. The pulse energy density is calculated by dividing the pulse energy by the area of the beam cross section on the surface of the object to be processed. Relatively large crystal grains are formed in the band-shaped region 7, and these crystal grains are connected in the long axis direction. These crystal grains have a length in the minor axis direction of about 1.5 to about and a size in the major axis direction of about 0.7 to about. The region 8 between the two band-like regions 7 forms a plurality of microcrystalline particles. Further, in the region 12 further outside the band-like region 7, there are crystal grains larger than the micro-crystal grains in the region 8, and crystal grains smaller than the crystal grains in the band-like region 7 are randomly arranged. By microscope observation, the boundaries of these areas can be detected as color differences. Next, we will examine the mechanism of crystal grains of various sizes as shown in Fig. -11-1240957 (8). Figure 4A shows the temperature dependence of the growth rate of silicon crystals, and Figure 4B shows the temperature dependence of the nucleation rate of non-crystal growth. The vertical axis in Figure 4a indicates the growth rate in units of 1 m / s, and the vertical axis in Figure 4b indicates the nucleation rate in units of "1 / c m3 · s". The horizontal axis of both is in units. "K" indicates temperature. The graphs of Figures 4A and 4B are obtained from the 22nd FEM Special Lecture Series of the Japan Plastics Processing Society's Analog Integrated Systems Branch, held on July 14, 1999 The method of "Micro-analysis of the crystal growth process of the movement of polycrystals" was published by Ichida Daichi (Sumitomo Heavy Industries, Ltd.) on pages 27 to 32. As shown in FIG. 4A, the growth rate at the melting point (; [6 8 3 κ) of single crystal silicon is 0, and the growth rate becomes faster as the temperature decreases. The growth rate is shown to be maximum at around 1 500K. Therefore, the lower the temperature of the molten silicon, the faster the crystal growth rate. The crystal growth rate also depends on the temperature gradient at the interface between the solid phase portion and the liquid phase portion. If the temperature gradient is steep, the crystal growth speed is fast. As shown in Fig. 4B, the nucleation rate increases from the melting point of silicon as the temperature decreases, and it is shown that the maximum temperature is around 600K. The band-like region 7 shown in FIG. 3 is considered to be a region having an appropriate temperature with a low nucleation rate and a fast growth rate, and an appropriate temperature gradient at the solid-liquid interface. The region 12 between the band-like region 7 and the amorphous region 9 has a higher nucleation rate because the temperature is lower than that of the band-like region 7, and the region has a slow growth rate because the temperature gradient at the solid-liquid interface is moderate. In this region, 'because many crystal nuclei are generated before growing into a large crystal', it cannot grow into large -12-1240957 (9) crystal grains. The microcrystalline region 8 is generally considered to be a region in which crystal nuclei are generated explosively by a decrease in temperature, and the crystal nuclei are formed to be more dominant than the crystal growth rate. When the temperature is cooled to a temperature at which the nucleation rate rapidly increases, the crystal growth in the band-shaped region 7 is hindered by newly generated crystal nuclei, and the crystal growth is stopped. Where crystal growth stops, it corresponds to the boundary between the band-like region 7 and the microcrystalline region 8. In more detail, in the area 12, it is generally considered that the crystal growth (heterogeneous growth) of the nucleus generated from the interface between the molten layer and its bottom layer is dominant, while in the microcrystalline area 8, it is derived from melting The crystal growth (homogeneous growth) of the nucleus generated inside the layer is dominant. Large crystal grains form at the boundary between the area dominated by heterogeneous growth and the area dominated by homogeneous growth. In order to form large crystal grains, it is necessary to prepare an appropriate temperature gradient and temperature of the molten portion of silicon with a fast growth rate and low nucleation rate. As shown in Fig. 2A, the temperature gradient at the position of the band-shaped region 7 is steep, and the region maintained at an appropriate temperature becomes narrower, and it is difficult to form large crystal grains. In order to form large crystal grains, it is preferable to make the gradient of the pulse energy density distribution near the band-like region 7 gentle. If the gradient of the pulse energy density distribution is too steep, the nucleation rate will increase. On the other hand, if the gradient of the pulse energy density distribution is too gentle, the crystal growth rate becomes slow. Therefore, it is generally considered that in order to form an appropriate temperature with a fast crystal growth rate and a low nucleation rate, and a temperature gradient at the solid-liquid interface, the gradient of the pulse energy density distribution must be not too steep and not too mild -13-1240957 (10) Appropriate range. Its / person 'will be described with reference to Fig. 5 on the pulse energy density distribution. Figure 5A is a graph showing the relationship between the crystal grain size and the beam width of the object to be processed. The horizontal axis represents light in the unit "# m" and the vertical axis represents the size of crystal grains in the unit "V m". The crystal grain calculation system uses the crystal growth S parity plan table disclosed in Japanese Patent Laid-Open Nos. 2000-1-2 9 7 9 8. The object to be processed is a silicon oxide film having a thickness of 100 nm, and an amorphous silicon film having a thickness of 5 nm is formed. For the pulsed thunder wavelength is 5 2 7nm, the pulse width (half chirp) is 14ns, and the incident area has a width of 1 W m on the outside of the half of the peak energy density, and 5 // on the inside. The total of m width is 6 // area for simulation. This is because the gradient of the pulse energy density distribution is almost the maximum at half of the peak, so large crystal grains are formed. The intensity distribution in the short-axis direction of the incident region of the light beam is distributed. For the four occasions where the width of the beam profile is 5.0 // m, 8 · 3 and // m, and 8 3.0 em, the peaks are strongly simulated, and the size of the crystal grains under the conditions of obtaining the largest crystal grains is determined as Crystal grain size at beam width. For the wide range of beam profile, 8.3 // m, 16.7 " m, and 83.0 / ^ m, the maximum density of each volume is U00mJ / cm2, 1 400 mJ / c mJ / cm2, and Under the condition of 1 5 00 mJ / cm2, the beam width of the surface with the best shape can be obtained. The knot revealed by the size meter and the position of the beam on the beam, and the position of the beam at m width shows the area shape. Gaussian: The mode of m and 16.7 degrees is at this light i 5.0 // m pulse energy η2, 1500 large crystals -14-1240957 (11)

J/JU 松c 第5 B圖係顯示在表示峰値強度之一半之値的位置的 脈衝能量密度分佈之梯度與結晶粒大小的關係圖。針對第 5 A圖之各評價點，計算脈衝能量密度分佈之梯度，作成 第5 B圖的圖形。 如第5 B圖所示，隨著脈衝能量密度分佈之梯度自2 0 m J / c m2 / // m開始增加，結晶粒逐漸變大。這是結晶生 長速度變快之故。然而，顯示在脈衝能量密度分佈之梯度 爲17 0mJ/ cm2 / // m附近結晶粒大小爲最大値，當梯度 大於此梯度時，結晶粒則變小。這是因爲脈衝能量密度之 梯度變陡峻，使固液界面的溫度梯度亦變得陡峻，且藉由 向橫方向的熱擴散使冷卻速度變快之故。亦即，這是並未 確保充分之結晶生長時間，造成在結晶生長成大結晶之前 ，產生多數的晶核的緣故。 製作第3圖所示之多結晶時之脈衝能量密度在5 0 0 mJ/cm2之位置的梯度係13mJ/cm2//im。有關第3圖 所示之帶狀區域7內之結晶粒之短軸方向的大小爲1 . 5〜2 // m左右，這與第5 B圖所示之模擬測試結果的傾向大致 相同。又，梯度爲18 之場合亦得到與第 5 B圖所示之模擬測試結果大致相同的傾向。如脈衝能量 密度在500 mJ/cm2之位置的梯度爲1〇 //m以 上’則可能得到與第5 B圖所示之模擬測試結果大致相同 的傾向。 由第5B圖所示之模擬測試結果判斷，爲形成大的結 •15- 1240957 (12) 晶粒，在第2 A圖以及第2 B圖所示之帶狀區域7之位置 (更嚴密而言，爲帶狀區域7的外側緣）的脈衝能量密度 分佈的梯度爲 2 8 0 m J / c m2 / # m以下較佳。此外，梯度 爲1 OmJ/ cm2/ // m以上較佳。又，將非結晶矽膜的厚度 作成1 0 0 n m進行同樣的模擬測試，仍會得到與厚度5 0 n m 之場合大致相同的傾向。 此外，第1實施例中，以第2 B圖所示方式，在結晶 粒隨機分佈之區域1 2使雷射光束之裙襬部之強度較高的 部分射入。藉由對區域1 2照射強度較高的雷射光束，使 該區域的溫度上昇。因此，帶狀區域7之溫度以及在固液 界面之溫度梯度會成爲滿足形成大的結晶粒的適當條件。 爲了要得到結晶粒增大之充分效果，將區域1 2之寬幅W 作成1 5 // m以上較佳。 其次，參照第6圖，就脈衝寬幅與結晶粒大小之關係 加以說明。 第6圖係顯示結晶粒大小與脈衝寬幅的關係圖。橫軸 以單位「ns」表示脈衝寬幅，縱軸以單位「// m」表示結 晶粒之大小。結晶粒大小之計算係採用上述之結晶成長評 價計畫表。 加工對象物、脈衝雷射光束之波長係與在第5圖說明 之條件相同。此外，在加工對象物表面之光束寬幅係作成 1 6.7 // m。模擬測試方法係與在第5圖說明之方法相同。 已知使脈衝寬幅變長則被形成之結晶粒會變大。這是 隨著脈衝寬幅變長而溫度降低會變緩和，結果，溶融部分 -16- 1240957 (13) 被維持在適當溫度的時間就會變長的緣故。然而，當脈衝 能量爲固定而加長脈衝寬幅時，會形成脈衝雷射光束之光 束強度降低，且無法維持足夠的能量密度。因而，脈衝寬 幅之上限係依所使用之雷射光源之輸出特性而受限制。 在使用準分子雷射作爲雷射光源之場合，一般而言脈 衝寬幅爲7〇ns以下。一般而言，Nd : YLF雷射等之全固 體雷射方面，有脈衝寬幅爲20〜30ns，或100ns以上的型 態。爲形成更大的結晶粒，使用脈衝寬幅爲1 00ms以上的 型態較佳。 以上，係爲了使矽溶融部分之溫度狀態成爲適當，而 著眼於脈衝能量密度分佈之形狀以及脈衝寬幅而進行的考 察，但藉由在脈衝雷射光束射入後，溶融部分完全固化之 前，使脈衝雷射光束再度射入相同位置，亦能控制溫度狀 態。 第7圖係圖不射入加工對象物之雷射光束的波形之一 例。橫軸表示經過時間，縱軸表示雷射光束之強度。在時 點t!使第1回之脈衝雷射光束s 1射入，在時點t2使第2 回之脈衝雷射光束S 2射入。第1回以及第2回之脈衝雷 射光束之脈衝寬幅（半値幅）分別係PW1以及PW2。第 7圖中顯示，第2回之脈衝雷射光束之峰値強度，爲小於 第1回之脈衝雷射光束之峰値強度之場合，但將兩者之峰 値強度作成相同亦可。 藉由第7圖所示之第1回之脈衝雷射光束S 1的射入 ’使非結晶矽膜溶融。溫度降低同時產生晶核，且從晶核 -17- 1240957 (14) 而結晶生長。在被冷卻至核生成率變大的溫度之前，使第 2回之脈衝雷射光束S2射入，進行再加熱。藉此，能抑 制晶核生成，使結晶生長繼續。因而，便能形成大的結晶 业丄 松。 例如，在利用第1回之射入而溶融的部分完全固化之 前，使第2回之脈衝雷射光束S 2射入亦可。例如將第1 回之雷射光束射入起至第2回之雷射光束射入爲止的遲延 時間設定在3 00〜1 5 00ns左右亦可。在使用全固體雷射作 爲雷射光源之場合，相較於使用準分子雷射之場合，能比 較容易控制遲延時間。又，如後述，暫時被形成之結晶粒 會比非結晶狀態之部分不易溶融。所以，暫時被形成之結 晶粒不易藉由第2次之脈衝雷射光束S2的照射而再溶融 〇 例如，射入脈衝能量密度之峰値爲1 3 00m cm2、脈 衝寬幅140ns、光束寬幅16.7 // m的脈衝雷射光束時的結 晶粒大小係約2.1 // m。相對於此，以第1回之脈衝能量 密度之峰値1 3 00 mJ/ cm2、第2回之脈衝能量密度之峰 値700 mJ/ cm2、遲延時間900ns之條件下進行多結晶化 後，結晶粒之大小則約4.4 // m。以此方式，便能藉由設 定遲延時間使第2次之脈衝雷射光束射入，以增大結晶粒 〇 將在藉由第1次之射入而溶融的部分固化之前照射第 2次之脈衝雷射光束的方式稱爲雙循衝（double-pUlse ) 方式。更爲一般而言，將在溶融的5夕固化之則照射第2回 -18- 1240957 (15) 以上之脈衝雷射光束的方式稱作多脈衝（muhi-Pulse ) 式。 依照上述第1實施例之方法中’並未使用用以將雷 光束之強度作成頂平（top flat )的光罩。因此’可提 雷射光束之能量利用效率。 此外，藉由上述第1實施例之方法，可形成結晶粒 第1方向連接成一列的結晶粒列。可以將有關與第1方 垂直之方向的結晶粒的平均大小作成1 ·5 A m以上。 其次，針對將以依照上述第1實施例之方法被形成 結晶粒朝基板面內方向進而擴大之第2實施例加以說明 第8圖係圖示模式化結晶生長之狀況。第8 A〜8 G 各圖係表示矽膜之剖面，圖之橫方向則相當於脈衝雷射 束之射入區域的短軸方向。 以第8A圖所示方式，當以依照上述第1實施例之 法使脈衝雷射光束射入，則在2條帶狀區域7之位置會 成連接在長軸方向之（在第8圖紙面垂直之方向）多數 結晶粒。在被挾於2個帶狀區域7之區域8會形成微結 粒。帶狀區域7之各個寬幅爲例如4 // m。以第5 A以 5 B圖所示方式，藉由使雷射光束之射入條件適當化， 以$形成大小4 // m左右之結晶粒。 第8B圖顯示使雷射光束之射入位置朝短軸方向移 1 5 // m，且進行第2回之照射後的結晶化狀態。例如， 束寬幅爲100/im、移動距離爲l5//m時，重疊率成爲 方 射 局 在 向 之 〇 圖 光 方 形 個 晶 及 足 動 光 -19- 85 (16) 1240957 在使帶狀區域7朝移動方向僅移動1 5 // m 形成結晶粒連接之帶狀區域2 0。帶狀區域2 〇之 β m。被挾在2個帶狀區域2 0之區域的非結晶 結晶粒，以及小的結晶粒會溶融，但如後述，帶 內之大結晶粒並不易溶融。實際上，帶狀區域7 粒係部分溶融，而另一部份則有結晶殘留。隨著 ，在帶狀區域7內殘留之結晶粒會成爲種晶，產 長。 假設發生與在第1回之照射下產生的結晶粒 程度的結晶生長，則在帶狀區域7之兩側生長之 度會成爲4#m左右。因此，以位於移動方向之 帶狀區域7作爲中心，會形成寬幅1 2 # m左右 區域7a。帶狀區域7a，與位於移動方向之前方 區域2 0之間的微結晶區域1 5的寬幅成爲約7 移動方向之後方側的帶狀區域7之周邊的非結晶 結晶粒，以及小的結晶粒因並未溶融，所以不會 生長。 第8C圖顯示使雷射光束之射入位置朝短軸 動1 5 &quot; m，且進行第3回之照射後的結晶化狀態 在使帶狀區域20朝移動方向僅移動15 // m 會形成結晶粒連接之帶狀區域2 1。帶狀區域2 1 m。再者，以帶狀區域7a以及位於移動方向 之帶狀區域20內的結晶粒作爲種晶，產生結晶生 從帶狀區域7a向移動方向之後方側，有約 的位置， 寬幅爲4 矽膜、微 狀區域7 內的結晶 溫度降低 生結晶生 大小相同 結晶的長 前方側的 的多結晶 側的帶狀 m。位於 矽膜、微 產生結晶 方向再移 〇 之位置， 之寬幅爲 之前方側 長。 4 // m 的 -20- 1240957 (17) 結晶生長。同時，從帶狀區域2 〇向移動方向之前方側， 有約4〆m的結晶生長。在被挾於帶狀區域7 a與帶狀區 域2 0之區域1 5，從兩側向中心產生結晶生長。因爲區域 1 5的覓幅係約7 m，所以在從兩側各生長3 . 5 # m之時 間點下，結晶粒們會產生接觸，且停止結晶生長。 藉此’形成包含帶狀區域7a之寬幅19.5/im的帶狀 區域7b，且形成包含帶狀區域20之寬幅11.5//m的帶狀 區域20a。在帶狀區域7b以及20a內，形成連接在長軸 方向之多數個結晶粒。沿著區域1 5之中心線1 6配列結晶 粒界。又，因爲結晶粒們產生接觸，而在中心線1 6的位 置形成山脈狀的凸部。 第8D圖顯示使雷射光束之射入位置朝短軸方向再移 動1 5 // m，且進行第4回照射後的結晶化狀態。 在使帶狀區域21朝移動方向之前方僅移動15//m的 位置形成帶狀區域22。以帶狀區域20a內的結晶粒作爲 種晶，在移動方向之前方側使結晶生長’以帶狀區域2 1 內的結晶粒作爲種晶，在其兩側使結晶生長。藉此’形成 寬幅15// m之帶狀區域20b以及寬幅11.5// m之帶狀區 域 2 1 a 〇 第8 E〜8 G圖分別顯示使雷射光束之射入位置朝短軸 方向僅移動1 5 // m，且進行第5〜7回照射後’的結晶化 狀態。 藉由第5回的照射’產生新的帶狀區域23，同時擴 大帶狀區域21a以及22’形成帶狀區域21b以及22a。藉 -21 - 1240957 (18) 由第6回的照射，擴大帶狀區域22a以及23，形成帶狀 區域22b以及23a。藉由第7回的照射，擴大帶狀區域 2 3 a，形成帶狀區域2 3 b。 如此’藉由使雷射光束之射入位置朝短軸方向移動同 時反覆進行照射，能使非結晶矽膜幾乎全面多結晶化。 第9圖顯示描繪以第8圖所示方法製作之多結晶膜的 SEM攝影。觀察複數之帶狀區域25。各帶狀區域25的寬 幅約爲在帶狀區域25內會形成在長軸方向上連 接之多數的結晶粒。在相互比鄰之帶狀區域2 5的邊界會 形成山脈狀的突起2 6。 其次，參照第1 〇圖，就用以全面多結晶化之條件加 以說明。縮小使脈衝雷射光束之射入位置移動時的重疊率 ，會擴大第8圖所示之微結晶區域1 5的寬幅，且在從區 域1 5之兩側開始生長之結晶粒們產生接觸之前，造成雷 射光束之射入區域偏離區域1 5。此外，即使保持固定之 重疊率，也會產生相同現象使每1次照射的結晶生長的長 度變短。因此，在每1回照射的結晶生長的長度短的場合 ，就必須提高重疊率。 第1 〇圖顯示每1次照射之結晶生長的長度與必要之 重疊率的關係圖。橫軸以單位^ # m」表示每1回照射之 結晶生長的長度，縱軸以單位「％」表示重疊率。由此可 知，例如，當每1次照射之結晶生長的長度爲1 〇 // m時 ，重疊率爲70%以上較佳。當每1次照射之結晶生長的 長度變短時，爲使全面多結晶化則須提高必要之重疊率。 -22- 1240957 (19) 爲使全面多結晶化，可以在從第8 B圖所示之微結晶 區域1 5之兩側開始生長的結晶粒們生長至產生接觸爲止 ’以微結晶區域1 5之中心線1 6位於利用雷射光束照射導 致之矽之溶融區域內之方式，設定重疊率。 其次’參照第1 1圖，針對非結晶矽膜多結晶化之場 合的雷射光束之較佳波長加以說明。 第1 1圖顯示非結晶矽與單結晶矽的光吸收係數之波 長依存性。橫軸係以單位「nm」表示波長，縱軸則以單 位「xl07cm_1」表示吸收係數。圖中的黑圈以及白圈係分 別顯示單結晶矽的吸收係數以及非結晶矽的吸收係數。 可知，在波長約3 4 Onm以上的區域，非結晶矽的吸 收係數大於卓結晶砂的吸收係數。特別是在波長4 0 0 n m〜 6 OOiim的範圍’非結晶矽的吸收係數會大於單結晶矽的吸 收係數1 0倍以上。在以暫時被形成之結晶粒作爲種晶進 行結晶生長的場合，不使結晶粒溶融而使非結晶區域溶融 較佳。實際上被形成之結晶粒分佈區域並非單結晶而是多 結晶。多結晶矽的吸收係數係依存於結晶粒的大小，吸收 係數在單結晶與非結晶之間。如結晶粒大，則接近單結晶 的吸收係數，結晶粒小，則接近非結晶的吸收係數。 因此，由於並不使第2B圖所示的帶狀區域7內的大 結晶粒溶融，而使非結晶區域9、隨機分佈區域1 2、以及 微結晶區域8優先溶融，所以使用波長3 40nm以上的脈 衝雷射光束較佳。因爲波長過長吸收係數會降低，所以將 使用的脈衝雷射光束的波長設定在900nm以下較佳。 -23- 1240957 (20) 在準分子雷射的波長區（約3 0 8 n m )，非結晶 收係數會局於波長在3 4 0〜9 0 0 n m的吸收係數。因 在非結晶矽膜的表面附近產生吸收，有關厚度方向 溫度梯度。相對地，如使用波長3 4 0〜9 0 0 n m的雷 ，雷射光束會侵入至非結晶矽膜的比較深的區域， 度方向則幾乎均等地被加熱。因此，能形成更高品 晶。 其次，參照第12圖，針對依照第3實施例之 膜之製造方法加以說明。 第12A圖顯示有關照射之雷射光束之短軸方 衝能量密度分佈與多結晶化區域的關係圖。脈衝能 最高的部分在射入區域3 5內形成微結晶，在其兩 大結晶粒於長軸方向連接之帶狀區域30A以及30B 成微結晶粒的區域3 5的寬幅與帶狀區域3 0 A以及 個的寬幅幾乎相等的方式來設定光束寬幅。 使雷射光束的射入位置朝短軸方向僅移動與帶 3 0 A之寬幅相等的距離後進行第2次雷射照射。 如第1 2B圖所示，在已經形成結晶粒的帶狀區 與3 0 B之間，形成大結晶粒連接的帶狀區域3〗A。 在位於移動方向之前方側的帶狀區域3 0B之前方側 帶狀區域3 1 B。 如此方式，利用2次照射，形成4個帶狀區域 31A、30B以及31B。相互比鄰之帶狀區域內的結 會相互接觸。藉由反覆進行同樣的工程，可使全面 矽的吸 此，僅 則產生 射光束 有關厚 質的結 多結晶 向的脈 量密度 側形成 。以形 30B各 狀區域 域3 0A 同時， ，形成 30A、 晶粒們 多結晶 -24- (21) 1240957 化° 又，隨著溫度條件不同，亦會有並非由第1 2 A圖所 示之區域3 5內產生的晶核新生長結晶粒，而是以兩側之 帶狀區域3 0 A以及3 0B內之結晶粒作爲種晶，而產生結 晶生長。 其次，參照第1 3圖，針對依照第4實施例之多結晶 膜之製造方法加以說明。 第1 3 A圖顯示有關照射之雷射光束之短軸方向的脈 衝能量密度分佈與多結晶化區域的關係圖。在對應於脈衝 能量密度之最高値的位置之兩側，形成大結晶粒於長軸方 向連接之帶狀區域36A以及36B。因爲光束寬幅狹窄，所 以帶狀區域3 6 A內之從晶核開始產生之結晶粒，與帶狀 區域3 6 B內之從晶核開始產生之結晶粒會相互接觸。沿著 兩者接觸的線3 8，進行結晶粒界配列。 僅以帶狀區域36A與36B合計的幅度，使雷射光束 的射入位置朝短軸方向移動，進行第2次照射。 如第1 3 B圖所示，形成相互鄰接之帶狀區域3 7 A與 3 7 B。位於移動方向之後方側的帶狀區域3 7 A會鄰接在第 1次照射下被形成之位於移動方向之前方側的帶狀區域 3 6B。藉由反覆進行同樣之工程，可使全面多結晶化。 藉由將第3以及第4實施例中照射之脈衝雷射光束之 脈衝能量密度分佈設定成第1實施例中說明之適當形狀， 可形成大結晶粒。此外，如第7圖所示，藉由對相同位置 使脈衝雷射光束射入2次，能產生更大的結晶粒。 -25- (22) 1240957 其次，參照第1 4圖〜第1 5 C圖，針對依照第5實施 例之多結晶膜之製造方法加以說明。 第1 4圖顯示處理對象物1之雷射光束射入位置附近 的剖面圖，以及有關光束剖面之短軸方向的脈衝能量密度 的分佈圖。一般而Η，脈衝能量密度係利用脈衝能量除以 光束剖面的面積而求得。以該計算求出之脈衝能量密度， 嚴密而言，爲光束剖面內的平均値。因爲光束剖面內的光 強度並非固定，所以脈衝能量密度亦並非固定。光強度分 佈近似於高斯分佈之場合，脈衝能量密度分佈亦近似於高 斯分佈。 如第1 4圖所示，處理對象物，參照第2 Α圖並與已 說明之第1實施例之場合相同，係在玻璃基板2上層積氧 化矽膜3、以及非結晶矽膜4的層積基板。脈衝雷射光束 之射入位置朝第14圖右方移動。 通過第1圖所示之均質器72的雷射光束之一部分會 被遮光板18遮光，透過成像光學裝置19而射入非結晶矽 膜4。遮光板1 8係遮住有關光束剖面之短軸方向的脈衝 能量密度分佈之裙襬部部分的光。成像光學裝置1 9係使 配置遮光板1 8的位置的光束剖面成像在非結晶矽膜4表 面。成像倍率爲例如1倍。 在未配置遮光板1 8之場合，在非結晶矽膜4表面之 有關脈衝雷射光束之短軸方向的脈衝能量密度的分佈係近 似於高斯分佈。亦即，脈衝能量密度形成在中央部強，而 愈接近邊緣愈弱。又，脈衝能量密度的分佈並非必須爲高 -26- (23) 1240957 斯分佈，一般而言，在中央部強，愈接近邊緣愈弱的分佈 亦可。 脈衝雷射光束之射入位置的行進方向之後方側之裙襬 部之中，脈衝能量密度在Eh以下的部分會被遮光板1 8遮 光，前方側方面則是脈衝能量密度在E l以下的部分會被 遮光。脈衝能量密度El係低於Eh。 實際上，在被遮光板1 8遮光的光束剖面之邊緣光強 度並不會立即變成〇，光束剖面會比被遮光之位置再朝外 側擴大6 // m左右。又，光束剖面的邊緣會位在光強度成 爲峰値的20%之處。 使具有此型態之脈衝能量密度分佈的脈衝雷射光束對 非結晶矽膜4射入1次。使非結晶矽膜4完全溶融之閾値 以上的脈衝能量密度之雷射光束會讓被照射的區域溶融。 脈衝能量密度EL在該閾値以上的場合，被脈衝雷射光束 照射的全部區域會溶融。在溶融部分被冷卻時，結晶會從 溶融部分的邊緣向內部生長。 如第1 5 A圖所示，在脈衝雷射光束之射入位置的移 動方向之後方側緣，會形成配列在光束剖面之長軸方向的 多數之結晶粒1 〇 〇 a，在前方側緣形成多數之結晶粒1 〇 1 a 。在形成結晶粒1 〇〇a之區域與形成結晶粒1 〇 1 a之區域所 挾的區域，與第3圖所示之區域8同樣地，會形成微結晶 粒。結晶生長的長度係依存於溶融部分的溫度與在固液界 面的溫度梯度。在後方側緣的溫度以及溫度梯度，與在前 方側緣的溫度以及溫度梯度爲互異。因此，從溶融之區域 -27- 1240957 (24) 的兩側緣開始生長的結晶之長度爲互異。 在後方側緣的溫度以及溫度梯度，在對結晶生長較佳 之條件的場合，於後方側緣形成之結晶粒1 〇〇a會大於在 前方側緣形成之結晶粒1 〇 1 a。例如，在後方側緣形成之 結晶粒1 〇 〇 a的橫方向尺寸可以達7〜8 // m。 其次，使脈衝雷射光束之射入位置朝光束剖面之短軸 方向移動，使脈衝雷射光束射入1次。射入位置的移動距 離係設定成新照射脈衝雷射光束的光束剖面的後方側緣會 鄰接或者重疊於結晶粒1 〇 〇 a的距離。前次照射時在前方 側緣形成之結晶粒1 〇 1 a係利用此次照射而溶融。 如第1 5 B圖所示，在此次照射下溶融之區域的後方側 緣，以結晶粒1 〇〇a作爲種晶朝橫方向使結晶生長，形成 內包結晶粒l〇〇a之大的結晶粒100b。此次照射之脈衝雷 射光束之光束剖面的後方側緣鄰接到結晶粒1 00a之場合 ，結晶粒100b之橫方向的尺寸成爲14〜16 &quot; m約爲結晶 粒I 0 0 a之尺寸的2倍。 脈衝雷射光束的射入位置，以前次射入而被照射之區 域與此次射入而被照射之區域會部分地重疊的方式移動， 同時反覆進行脈衝雷射光束的照射。移動距離係設定成新 照射脈衝雷射光束的光束剖面的後方側緣會鄰接或者重疊 於前次照射下形成之後方側的結晶粒的距離。 如第1 5 C圖所示，結晶粒朝橫方向生長，形成大的結 晶粒100c。於第15B圖的時點下，在光束剖面之前方側 緣已經形成之小的結晶粒1 0 1 b係利用之後的脈衝雷射光 -28- 1240957 (25) 束的照射而溶融，並消滅。 第5實施例中，結晶會從以遮光板1 8劃定之光束剖 面的後方側緣開始生長。在第1實施例的場合，如第3圖 所示產生大結晶粒之帶狀區域7爲蛇行形狀。第5實施例 中，因爲結晶粒1 00a之形成位置係利用遮光板1 8以人爲 方式決定，所以結晶粒1 00a連接之帶狀區域並非蛇行形 狀，而是幾乎沿著直線的形狀。因此，在第2次照射時， 光束剖面之後方側緣能以鄰接結晶粒1 00a連接之帶狀區 域的方式容易定位。 此外，結晶生長的方向亦一致朝垂直於光束剖面之長 軸的方向。在多結晶膜形成主動元件的場合，藉由使形成 之主動元件之電流方向平行於結晶生長之方向，能抑制結 晶粒界所造成之載子移動度降低。 上述實施例中，每次使脈衝雷射光束射入1次下，都 使射入位置移動，以參照第7圖說明的方式，採用對相同 位置使脈衝雷射光束射入2次的雙脈衝方式亦可，採用多 脈衝方式亦可。藉此，能增大形成之結晶粒。 第1 4圖所示之脈衝能量密度分佈之裙襬部之中應該 遮光之較佳區域，亦即脈衝能量密度Eh以及EL之較佳大 小可藉由變動遮光區域之大小（寬幅）進行複數之評價實 驗而求得。 以下，針對實際進行之評價實驗的結果加以說明。從 雷射光源射出的雷射光束會形成具有寬幅100#m'長度 1 7 mm之光束剖面的長尺寸光束。將該光束剖面之寬幅方 -29- 1240957 (26) 向兩側以遮光板遮光，做成寬幅2 2 &quot; m之剖面形狀，使 該光束剖面成像於非結晶矽膜表面。又，光束剖面之寬幅 係光強度分佈之半値幅。 使用2台雷射光源，並採用將第1次以及第2次脈衝 雷射光束之在非結晶矽膜表面之脈衝能量密度分別設定成 550 mJ/cm2以及500 mj/cm2，將遲延時間設定成100ns 的雙脈衝方式。 該條件下，利用照射2次脈衝雷射光束，在光束剖面 之掃瞄方向後方側形成的結晶粒1 〇〇a之寬幅會成爲3 · 1 // m。以3 // m的間距使脈衝雷射光束射入的方式掃瞄非結 晶矽膜之表面，如第1 5 C圖所示，能在掃瞄方向使結晶連 續地生長。在測定各結晶粒之配向性之際，各結晶粒之〈 1 1 〇〉方向會一致朝與結晶生長方向（掃瞄方向）平行之 方向。 其次，參照第1 6圖〜第1 7 C圖，針對依照第6實施 例之多結晶膜之製造方法加以說明。 如第1 6圖所示’第6實施例中，在脈衝雷射光束之 射入位置的移動方向之前方側，將脈衝能量密度在Eh以 下的裙襬部之部分以遮光板1 8遮光，在後方側，將脈衝 能量密度在el以下的裙襬部之部分以遮光板1 8遮光。 如第1 7 A圖所示，進行1次照射之際，在光束剖面 之前方側緣會形成較大的結晶粒1 1 0a，而在後方側緣形 成較小的結晶粒1 1 1 a。 如第1 7B圖所示’使脈衝雷射光束之射入位置移動並 -30- (27) 1240957 進行下〗次照射之際，會形成結晶粒1 1 Ob以及1 1 1 b。由 於較大的結晶粒Π 〇a不易溶融’所以在下次之後的照射 都幾乎不會溶融。結晶粒1 1 Ob係從溶融之區域的前方側 緣向後方側（結晶粒1 1 〇a側）生長。在結晶生長的先端 抵達結晶粒11 之時點下生長會停止。 此時，亦會產生將已經形成之結晶粒1 1 0a作爲種晶 並朝橫方向生長之結晶。因此，脈衝雷射光束之射入位置 的移動距離可以比結晶粒1 1 的寬幅還長。 如第1 7C圖所示，使脈衝雷射光束之射入位置移動同 時反覆進行照射之際，會形成較大的結晶粒1 1 〇a〜1 1 0e 。此外，第1 7 C圖中，在第3次照射時，在光束剖面之後 方側緣會形成較小的結晶粒1 1 1 c。在第4次以後的照射 ，因爲光束剖面之後方側緣變成位於較大的結晶粒1 1 〇a 〜1 1 〇e的內部，所以在後方側緣附近並不會發生溶融部 分。 第6實施例中，如第1 7C圖所示，例如在結晶粒 ll〇a連接之帶狀區域與結晶粒110b連接之帶狀區域之間 會形成明確的邊界。該邊界之位置係藉遮光板1 8人爲決 定。例如，在多結晶化之矽薄膜形成主動元件之場合，可 以主動元件未跨過結晶粒之邊界的方式，配置結晶粒之邊 界。如以上方式，可如第9圖所示以帶狀區域覆蓋基板全 部。 以下，針對實際進行之評價實驗的結果加以說明。從 雷射光源射出的雷射光束會形成具有寬幅100//m、長度 -31 - 1240957 (28) 1 7 m m之光束剖面的長尺寸光束。將該光束剖面之掃瞄方 向前方側緣以遮光板遮光，做成寬幅5 y m之剖面形狀， 使該光束剖面成像於非結晶矽膜表面。使用2台雷射光源 ，並採用將第1次以及第2次脈衝雷射光束之在非結晶矽 膜表面之脈衝能量密度分別設定成710 mJ/ cm2以及 6 4 0 m J / c m 2，將遲延時間設定成2 0 0 n s的雙脈衝方式。 該條件下，利用照射2次脈衝雷射光束，在光束剖面 之掃瞄方向前方側形成的結晶粒1 0 0 a之寬幅會成爲5 · 4 m。以1 2 // m的間距使脈衝雷射光束射入的方式掃瞄非結 晶矽膜之表面，能在光束剖面之長邊方向形成結晶粒連接 之寬幅1 2 m的帶狀區域。相互比鄰之帶狀區域的結晶 粒會在帶狀區域之邊界相互接觸，且全面多結晶化。 不論1次照射下形成之結晶粒1 l〇a之寬幅是否爲5.4 m，最終形成之帶狀區域之寬幅都會成爲1 2 // m，這是 將1次照射下形成之寬幅5.4 // m的結晶粒作爲種晶，利 用之後的照射會在橫方向產生結晶生長之故。該生長過程 與在第8 A圖〜第8 G圖已說明之結晶生長過程相同。 上述第5以及第6實施例之評價實驗中，係採用雙脈 衝方式。此時，將從第1次脈衝雷射光束射入起至第2次 脈衝雷射光束射入爲止的遲延時間設定爲1〇〇〜l〇〇〇ns較 佳。該適當之遲延時間會稍微短於未採用遮光板之場合下 的遲延時間。這是在光束剖面之兩側光強度分佈的傾斜陡 峻，固化速度比未採用遮光板之場合下還快速之故。 其次，就第7實施例加以說明。第5以及第6實施例 -32- 1240957 (29) 中，有關光束剖面之橫寬方向以使光強度分佈（或者脈衝 能量密度分佈）形成非對稱的方式，將雷射光束之_部# 以遮光板遮光，但以形成對稱的方式遮光亦可。如光強度 分佈成爲對稱，在掃瞄方向之前方側緣與後方側緣會形成 幾乎相同大小之結晶粒。因此，利用與依參照第8 A圖〜 桌8G圖說明之第2貫施例，參照第12A圖以及第12B圖 說明之第3實施例，或者參照第1 3 A圖以及第1 3 B圖說 明之第4實施例之方法相同的方法，可進行非結晶矽膜的 多結晶化。 上述第5〜第7實施例中，使配置遮光板之位置的光 束剖面成像於非結晶矽膜表面，但使遮光板配置接近於非 結晶矽膜亦可。遮光板與非結晶矽膜之間隔係例如可以做 成0 . 1 mm左右。 上述第1以及第6實施例中，藉由將雷射光束之一部 分以遮光板遮光’形成有關光束剖面之寬幅方向具有非對 稱之光強度分佈的雷射光束，但利用其他光學裝置將光強 度分佈做成非對稱亦可。例如，將在石英玻璃表面配置鉻 (C〇等之點狀圖案的梯度濾光器配置在光路內亦可。 依循以上實施例說明本發明，但本發明並未侷限於此 。例如，業者當然可進行種種可能的變更、改良、組合等 【圖式簡單說明】 第1圖係實施例中使用之雷射退火裝置的槪略平面圖 -33- 1240957 (30) 第2A圖係加工對象物的剖面圖，以及顯示第1實施 例中使用之脈衝雷射光束之，在加工對象物表面的脈衝能 量密度分佈圖，第2 B圖係被多結晶化之加工對象物的模 式平面圖。 第3圖係描繪依照第1實施例之方法所製作之多結晶 膜的SEM攝影。 第4A圖係顯示溶融之矽的溫度與結晶生長速度的關 係圖，第4B圖係顯示溫度與核生成率的關係圖。 第5 A圖係顯示光束剖面之寬幅與結晶粒大小的關係 圖’第5 B圖係顯示脈衝能量密度分佈之梯度與結晶粒大 小的關係圖。 第6圖係顯示脈衝寬幅與結晶粒大小的關係圖。 第7圖係圖示對1處使脈衝雷射光束2次照射之場合 之’雷射光束波形之一例。 第8圖係模式化圖示依照第2實施例之多結晶膜之製 造方法的製造途中的薄膜剖面。 第9圖係描繪依照第2實施例之方法所製造之多結晶 膜的S E Μ攝影。 第1 〇圖係顯示每1回照射之結晶生長之長度，與爲 使全面多結晶化所必要之重疊率的關係圖。 第1 1圖係圖示單結晶矽與非結晶矽之吸收係數之波 長依存性。 第1 2 Α圖係顯示依照第3實施例之多結晶膜之製造 -34- (31) 1240957 方法下使用之脈衝雷射光束之脈衝能量密度分佈與多結晶 化區域的關係圖，第1 2 B圖係被製造之多結晶膜之模式平 面圖。 第1 3 A圖係顯示依照第4實施例之多結晶膜之製造 方法下被使用之脈衝雷射光束之脈衝能量密度分佈與多結 晶化區域的關係圖，第1 3 B圖係被製造之多結晶膜之模式 平面圖。 第1 4圖係顯示依照第5實施例之多結晶膜之製造方 法採用之處理對象基板與遮光板的剖面圖，以及脈衝能量 密度的分佈圖。 第15A〜15C圖係用以顯示依照第5實施例之多結晶 膜之製造方法進行多結晶化的槪略圖。 第1 6圖係顯示依照第6實施例之多結晶膜之製造方 法採用之處理對象基板與遮光板的剖面圖，以及脈衝能量 密度的分佈圖。 第1 7 A〜1 7 C圖係用以顯示依照第6實施例之多結晶 膜之製造方法進行多結晶化的槪略圖。 圖號說明 40 處理室 44 平臺 6〇 滑動機構 6 3、6 5 結合構件 64 線性導引機構 -35- 1240957 66 (32) 線性馬達 67 伸縮軟管 7 1 雷射光源 72 均質器 82 搬送室 83 . 84 搬出入室 85、 86、87 閘閥 88 C C D攝影器 89 錄影監視器 94 搬送用機器手臂 -36-J / JU Songc Figure 5B is a graph showing the relationship between the gradient of the pulse energy density distribution and the crystal grain size at a position representing half of the peak chirp intensity. For each evaluation point in Fig. 5A, the gradient of the pulse energy density distribution is calculated, and the graph in Fig. 5B is prepared. As shown in Fig. 5B, as the gradient of the pulse energy density distribution increases from 20 m J / c m2 / // m, the crystal grains gradually become larger. This is because the crystal growth speed becomes faster. However, it is shown that the gradient of the pulse energy density distribution is about 170 mJ / cm2 // m, and the size of the crystal grains is the largest. When the gradient is larger than this gradient, the crystal grains become smaller. This is because the gradient of the pulse energy density becomes steeper, the temperature gradient at the solid-liquid interface becomes steeper, and the cooling rate becomes faster by thermal diffusion in the lateral direction. That is, this is because sufficient crystal growth time is not ensured, and a large number of crystal nuclei are generated before the crystal grows into a large crystal. The gradient of the pulse energy density at the position of 500 mJ / cm2 at the time of making the polycrystal shown in Fig. 3 is 13 mJ / cm2 // im. The size of the minor axis direction of the crystal grains in the band-like region 7 shown in Fig. 3 is 1.  5 ~ 2 // m, which is roughly the same as the tendency of the simulated test results shown in Figure 5B. When the gradient is 18, a tendency similar to that of the simulation test result shown in Fig. 5B is obtained. If the gradient of the pulse energy density at a position of 500 mJ / cm2 is 10 / m or more ', a tendency similar to that of the simulation test result shown in Fig. 5B may be obtained. Judging from the simulation test results shown in Figure 5B, in order to form a large junction • 15-1240957 (12) grains, the position of the band-shaped area 7 shown in Figure 2A and Figure 2B (more tight and In other words, the gradient of the pulse energy density distribution at the outer edge of the strip-shaped region 7 is preferably 280 m J / c m2 / # m or less. In addition, a gradient of 1 OmJ / cm2 / // m or more is preferable. In addition, when the thickness of the amorphous silicon film was set to 100 nm and the same simulation test was performed, the same tendency as that in the case of a thickness of 50 nm was obtained. In addition, in the first embodiment, as shown in Fig. 2B, in the region 12 where the crystal grains are randomly distributed, the portion with a higher intensity of the skirt portion of the laser beam is incident. The area 12 is irradiated with a laser beam having a relatively high intensity, thereby increasing the temperature in the area. Therefore, the temperature of the band-like region 7 and the temperature gradient at the solid-liquid interface become suitable conditions for forming large crystal grains. In order to obtain a sufficient effect of increasing the crystal grains, it is preferable to make the width W of the region 12 to 15 / m or more. Next, the relationship between the pulse width and the crystal grain size will be described with reference to FIG. Fig. 6 is a graph showing the relationship between crystal grain size and pulse width. The horizontal axis represents the pulse width in the unit "ns", and the vertical axis represents the size of the junction grains in the unit "// m". The crystal grain size is calculated using the above-mentioned crystal growth evaluation plan. The wavelengths of the object to be processed and the pulsed laser beam are the same as those described in FIG. 5. In addition, the beam width on the surface of the object to be processed is made 16. 7 // m. The simulation test method is the same as the method illustrated in FIG. It is known that as the pulse width becomes longer, the crystal grains formed become larger. This is because the temperature decreases as the pulse width becomes longer, and as a result, the time for which the melting part -16-1240957 (13) is maintained at an appropriate temperature becomes longer. However, when the pulse energy is fixed and the pulse width is lengthened, the beam intensity of the pulsed laser beam is reduced, and sufficient energy density cannot be maintained. Therefore, the upper limit of the pulse width is limited depending on the output characteristics of the laser light source used. When an excimer laser is used as the laser light source, the pulse width is generally less than 70ns. Generally speaking, for all solid-state lasers such as Nd: YLF lasers, there are pulse widths of 20 to 30 ns, or more than 100 ns. In order to form larger crystal grains, it is preferable to use a pulse width of 100 ms or more. The above is to investigate the shape of the pulse energy density distribution and the pulse width in order to make the temperature state of the molten portion of silicon appropriate. However, after the pulsed laser beam is injected and before the molten portion is completely solidified, The pulsed laser beam can be injected into the same position again, and the temperature state can also be controlled. Fig. 7 is an example of a waveform of a laser beam which is not incident on an object to be processed. The horizontal axis represents the elapsed time, and the vertical axis represents the intensity of the laser beam. At time t !, the first pulsed laser beam s1 is made incident, and at time t2, the second pulsed laser beam S2 is made incident. The pulse widths (half-width) of the first and second pulsed laser beams are PW1 and PW2, respectively. Fig. 7 shows that the peak chirp intensity of the second pulse laser beam is smaller than the peak chirp intensity of the first pulse laser beam, but the peak chirp intensity of the two may be made the same. The amorphous silicon film is melted by the injection of the first pulsed laser beam S 1 shown in FIG. 7. The crystal nucleus is generated at the same time as the temperature decreases, and the crystal grows from the crystal nucleus -17-1240957 (14). Before being cooled to a temperature at which the nucleation rate becomes large, the second pulsed laser beam S2 is made incident and reheated. This can suppress the formation of crystal nuclei and continue crystal growth. As a result, large crystals can be formed. For example, before the melted portion is completely cured by the first injection, the second pulse laser beam S 2 may be incident. For example, the delay time from the first laser beam to the second laser beam may be set to about 300 to 1500 ns. In the case of using an all-solid-state laser as a laser light source, it is easier to control the delay time than in the case of using an excimer laser. As will be described later, the crystalline particles that are temporarily formed are less likely to be melted than the non-crystalline portions. Therefore, the temporarily formed crystal particles cannot be easily re-melted by the irradiation of the second pulsed laser beam S2. For example, the peak pulse energy density 値 is 1 300m cm2, the pulse width is 140ns, and the beam width is 16. The grain size of the 7 // m pulsed laser beam is about 2. 1 // m. In contrast, the first pulse energy density peak 値 1 3 00 mJ / cm2, the second pulse energy density peak 値 700 mJ / cm2, and the delay time 900ns was used for polycrystallization, and then crystallized. The grain size is about 4. 4 // m. In this way, it is possible to make the second pulse laser beam incident by setting the delay time to increase the crystal grains. The second time will be irradiated before the part melted by the first injection is solidified. The pulsed laser beam method is called a double-pUlse method. More generally, a method of irradiating a pulse of a laser beam of -18-1240957 (15) or more for the second time when it is cured on the 5th of melting is called a multi-pulse (muhi-pulse) method. In the method according to the above-mentioned first embodiment, a photomask for making the intensity of a thunder beam into a top flat is not used. Therefore, 'the energy utilization efficiency of the laser beam can be improved. In addition, by the method of the first embodiment described above, crystal grain rows can be formed in which crystal grains are connected in a first direction in a row. The average size of crystal grains in a direction perpendicular to the first party can be made to be 1.5 mm or more. Next, a second embodiment will be described in which crystal grains formed by the method according to the first embodiment are expanded inwardly of the substrate, and FIG. 8 is a view showing a state of the patterned crystal growth. 8A to 8G each show a cross-section of a silicon film, and the horizontal direction of the figure corresponds to the short-axis direction of the incident area of the pulsed laser beam. In the manner shown in FIG. 8A, when the pulsed laser beam is made incident in accordance with the method of the first embodiment described above, the positions of the two strip-shaped regions 7 are connected in the direction of the long axis (on the eighth drawing surface). Vertical direction) Most crystal grains. Micro-grains are formed in the region 8 trapped in the two band-shaped regions 7. Each width of the strip-shaped region 7 is, for example, 4 // m. In the manner shown in Figures 5A and 5B, by optimizing the incident conditions of the laser beam, crystal grains with a size of about 4 // m are formed in $. FIG. 8B shows the crystallization state after the incident position of the laser beam is shifted in the direction of the short axis by 1 5 // m, and the second irradiation is performed. For example, when the beam width is 100 / im and the moving distance is 15 // m, the overlap ratio becomes the square beam and the square crystal and the foot moving light -19- 85 (16) 1240957 Zone 7 moves only 1 5 // m in the direction of movement to form a band-like zone 20 of crystal grains. Banded area 2 β m. Amorphous crystal grains and small crystal grains that are trapped in the two band-shaped regions 20 will melt, but as will be described later, the large crystal grains in the band are not easily melted. In fact, part of the 7 bands in the banded region melted, while the other part had crystals remaining. As the crystal grains remaining in the band-like region 7 become seed crystals, they grow. Assuming that crystal growth occurs to the extent that the crystal grains are generated under the first irradiation, the degree of growth on both sides of the band-shaped region 7 will be about 4 #m. Therefore, the belt-shaped region 7 located in the moving direction is used as the center, and a wide region 7a of about 1 2 #m is formed. The width of the band-shaped region 7a, and the microcrystalline region 15 located between the front-side region 20 and the front-side region 20 is approximately 7. The non-crystalline grains around the band-shaped region 7 on the side behind the direction of movement, and small crystals The grains do not grow because they do not melt. Fig. 8C shows that the position of the laser beam is moved toward the short axis by 1 5 &quot; m, and the crystallization state after the third round of irradiation moves the band-shaped region 20 in the moving direction only 15 // m will A band-like region 21 where crystal grains are connected is formed. Banded area 2 1 m. In addition, the crystal grains in the band-shaped region 7a and the band-shaped region 20 located in the moving direction are used as seed crystals to generate crystal growth from the band-shaped region 7a to the rear side of the moving direction. The crystallization temperature in the film and the micro-like region 7 decreases, and the crystalline m has the band-shaped m on the polycrystalline side of the long front side of the crystals of the same size. It is located at the position where the silicon film and the micro-crystallized direction are shifted by 〇, and the width is the front side length. 4 // m of -20- 1240957 (17) Crystal growth. At the same time, from the band-shaped area 20 to the front side of the moving direction, a crystal of about 4 μm grows. In the region 15 surrounded by the band-shaped region 7a and the band-shaped region 20, crystal growth occurs from both sides to the center. Because the foraging area of area 15 is about 7 m, it grows 3 on each side.  At 5 # m, the crystal grains will come into contact and stop crystal growth. Thereby, a wide 19 including a strip-shaped region 7a is formed. 5 / im strip-shaped region 7b, and a wide width 11 including the strip-shaped region 20 is formed. 5 // m strip-shaped region 20a. In the band-like regions 7b and 20a, a plurality of crystal grains connected in the major axis direction are formed. Crystal grain boundaries are aligned along the center line 16 of area 15. In addition, since the crystal grains come into contact with each other, a mountain-like convex portion is formed at the position of the center line 16. Fig. 8D shows the crystallization state after the incident position of the laser beam is further moved in the direction of the short axis by 15 / m and the fourth irradiation is performed. The band-shaped region 22 is formed by moving the band-shaped region 21 only 15 // m before the band-shaped region 21 is moved in the moving direction. The crystal grains in the band-shaped region 20a are used as seed crystals, and crystals are grown on the side before the moving direction. The crystal grains in the band-shaped region 21 are used as seed crystals, and crystals are grown on both sides thereof. Thereby, a band-shaped region 20b with a width of 15 // m and a width of 11. 5 // m band-shaped area 2 1 a 〇 The 8th E ~ 8G diagrams respectively show that the incident position of the laser beam is moved toward the short axis direction by only 1 5 // m, and after the 5th to 7th irradiation 'Crystalline state. A new band-like region 23 is generated by the fifth irradiation ', and the band-like regions 21a and 22' are enlarged at the same time to form the band-like regions 21b and 22a. Borrow -21-1240957 (18) By the sixth irradiation, the band-shaped regions 22a and 23 are enlarged to form the band-shaped regions 22b and 23a. By the seventh irradiation, the band-shaped region 2 3 a is enlarged to form the band-shaped region 2 3 b. In this way, by moving the incident position of the laser beam in the short-axis direction while irradiating it repeatedly, the amorphous silicon film can be almost polycrystallized. Fig. 9 shows an SEM photograph depicting a polycrystalline film produced by the method shown in Fig. 8. Observe a plurality of banded areas 25. The width of each of the band-shaped regions 25 is about a large number of crystal grains connected in the major axis direction in the band-shaped regions 25. Mountain-like protrusions 26 are formed at the borders of the adjacent strip-shaped regions 25. Next, referring to Fig. 10, the conditions for full polycrystallization will be explained. Decreasing the overlap rate when the incident position of the pulsed laser beam is moved will increase the width of the microcrystalline region 15 shown in FIG. 8 and contact the crystal grains that have grown from both sides of the region 15 Previously, the incident area of the laser beam was caused to deviate from the area 15. In addition, even if the overlap ratio is kept constant, the same phenomenon occurs, and the length of crystal growth per one irradiation is shortened. Therefore, when the length of crystal growth per irradiation is short, it is necessary to increase the overlap ratio. Figure 10 shows the relationship between the length of crystal growth per irradiation and the necessary overlap ratio. The horizontal axis represents the length of the crystal growth per irradiation with the unit ^ # m ", and the vertical axis represents the overlap ratio with the unit"% ". It can be seen from this that, for example, when the length of the crystal growth per one irradiation is 10m, the overlap ratio is preferably 70% or more. When the length of the crystal growth per one irradiation becomes short, it is necessary to increase the necessary overlap ratio in order to achieve full polycrystallization. -22- 1240957 (19) In order to fully crystallize, the crystal grains that grow from both sides of the microcrystalline region 15 shown in Fig. 8B can be grown until contact occurs. The center line 16 is set in such a manner that the overlap rate is set in such a manner that the silicon melt region is caused by laser beam irradiation. Next, referring to Fig. 11, the preferred wavelength of the laser beam in the field of polycrystalline silicon film polycrystallization will be described. Figure 11 shows the wavelength dependence of the light absorption coefficient of amorphous silicon and single crystal silicon. The horizontal axis represents the wavelength in the unit "nm", and the vertical axis represents the absorption coefficient in the unit "xl07cm_1". The black circles and white circles in the figure show the absorption coefficients of monocrystalline silicon and the absorption coefficients of amorphous silicon, respectively. It can be seen that the absorption coefficient of amorphous silicon is larger than the absorption coefficient of crystalline sand in a region with a wavelength of about 3 4 Onm or more. In particular, the absorption coefficient of amorphous silicon in a wavelength range of 400 nm to 600 μm is more than 10 times larger than that of single crystal silicon. When crystal growth is performed using the temporarily formed crystal grains as seed crystals, it is preferable not to melt the crystal grains but to melt the amorphous region. In fact, the distribution area of the crystal grains formed is not a single crystal but a polycrystal. The absorption coefficient of polycrystalline silicon depends on the size of the crystal grains, and the absorption coefficient is between single crystal and amorphous. If the crystal grains are large, the absorption coefficient is close to that of a single crystal, and when the crystal grains are small, the absorption coefficient is close to that of an amorphous crystal. Therefore, since the large crystal grains in the band-shaped region 7 shown in FIG. 2B are not melted, but the amorphous region 9, the randomly distributed region 12, and the microcrystalline region 8 are preferentially melted, the wavelength 3 or more is used. A pulsed laser beam is preferred. Since the absorption coefficient will decrease if the wavelength is too long, it is better to set the wavelength of the pulsed laser beam used below 900 nm. -23- 1240957 (20) In the wavelength region of the excimer laser (approximately 308 nm), the amorphous yield coefficient will be localized to the absorption coefficient at a wavelength of 3400 ~ 900 nm. Since absorption occurs near the surface of the amorphous silicon film, a temperature gradient in the thickness direction is involved. In contrast, if a laser with a wavelength of 340 to 900 nm is used, the laser beam will penetrate into a relatively deep area of the amorphous silicon film, and the degree direction will be almost uniformly heated. Therefore, higher crystals can be formed. Next, a method for manufacturing a film according to the third embodiment will be described with reference to FIG. Fig. 12A is a graph showing the relationship between the short-axis impact energy density distribution of the irradiated laser beam and the polycrystalline region. The part with the highest pulse energy forms microcrystals in the injection region 35, and in the band-shaped regions 30A and 30B where the two large crystal grains are connected in the long axis direction, the microcrystalline grain regions 3 5 are wide and the band-shaped regions 3 0 A and the widths of the beams are set in almost equal ways. After the incident position of the laser beam is moved in the short axis direction by a distance equal to the width of the band 30 A, the second laser irradiation is performed. As shown in Fig. 12B, between the band-shaped region where the crystal grains have been formed and 3 0 B, a band-shaped region 3A where large crystal grains are connected is formed. The band-shaped region 3 0B located on the side on the front side in the moving direction is the band-shaped area 3 1 B on the front side. In this manner, four band-shaped regions 31A, 30B, and 31B are formed by two irradiations. The knots in adjacent banded areas will contact each other. By performing the same process over and over again, it is possible to absorb the entire silicon, and only the pulse density of the thick junction polycrystalline direction of the beam is formed. In the shape of 30B, the various regions 3 0A. At the same time, 30A is formed, and the crystals are polycrystalline -24- (21) 1240957 °. Moreover, depending on the temperature conditions, there may be some not shown in Figure 12A The crystal nuclei generated in the region 35 are newly grown crystal grains, but the crystal grains in the band-shaped regions 30 A and 30 B on both sides are used as seed crystals to generate crystal growth. Next, a method for manufacturing a polycrystalline film according to the fourth embodiment will be described with reference to Figs. Fig. 1A shows the relationship between the pulse energy density distribution in the minor axis direction of the irradiated laser beam and the polycrystalline region. On both sides of the position corresponding to the highest chirp of the pulse energy density, band-shaped regions 36A and 36B in which large crystal grains are connected in the long axis direction are formed. Because the beam width is narrow, the crystal grains starting from the crystal nuclei in the banded region 3 6 A and the crystal grains starting from the crystal nuclei in the banded region 3 6 B will contact each other. Crystal grain boundary alignment is performed along the line 38 where the two are in contact. Only the width of the band-shaped regions 36A and 36B is used to move the incident position of the laser beam toward the minor axis, and the second irradiation is performed. As shown in Fig. 1B, adjacent band-shaped regions 3 7 A and 3 7 B are formed. The band-shaped area 3 7 A on the side behind the moving direction adjoins the band-shaped area 3 6B on the side before the moving direction formed under the first irradiation. By repeating the same process over and over, full polycrystallization can be achieved. By setting the pulse energy density distribution of the pulsed laser beams irradiated in the third and fourth embodiments to the appropriate shape described in the first embodiment, large crystal grains can be formed. In addition, as shown in Fig. 7, by pulsing the pulsed laser beam twice at the same position, larger crystal grains can be generated. -25- (22) 1240957 Next, a method for manufacturing a polycrystalline film according to the fifth embodiment will be described with reference to Figs. 14 to 15C. Fig. 14 shows a cross-sectional view near the incident position of the laser beam of the processing object 1, and a distribution diagram of the pulse energy density in the short-axis direction of the beam cross-section. Generally, the pulse energy density is obtained by dividing the pulse energy by the area of the beam cross section. The pulse energy density obtained by this calculation is, strictly speaking, the average chirp in the beam profile. Because the light intensity in the beam profile is not constant, the pulse energy density is also not constant. When the light intensity distribution is similar to the Gaussian distribution, the pulse energy density distribution is also similar to the Gaussian distribution. As shown in FIG. 14, the processing target is the same as that in the case of the first embodiment described with reference to FIG. 2A, and the silicon oxide film 3 and the amorphous silicon film 4 are laminated on the glass substrate 2.量 SUB BOARD. The incident position of the pulsed laser beam moves to the right in FIG. 14. A part of the laser beam passing through the homogenizer 72 shown in Fig. 1 is shielded by the light shielding plate 18, passes through the imaging optical device 19, and enters the amorphous silicon film 4. The light-shielding plate 18 shields the light in the skirt portion of the pulse energy density distribution in the short axis direction of the beam profile. The imaging optical device 19 images a beam cross section at a position where the light shielding plate 18 is disposed on the surface of the amorphous silicon film 4. The imaging magnification is, for example, 1 times. When the light shielding plate 18 is not provided, the distribution of the pulse energy density in the minor axis direction of the pulsed laser beam on the surface of the amorphous silicon film 4 is similar to a Gaussian distribution. That is, the pulse energy density is strong at the center, and becomes weaker as it approaches the edges. In addition, the distribution of the pulse energy density does not necessarily have to be a high -26- (23) 1240957 distribution, but in general, a distribution that is strong in the center and weaker as it approaches the edges is also acceptable. In the direction of travel of the position where the pulsed laser beam is incident, in the skirt portion on the side, the part with the pulse energy density below Eh is blocked by the light shielding plate 18, and the front side is where the pulse energy density is below E l Some will be blocked. The pulse energy density El is lower than Eh. In fact, the light intensity at the edge of the light beam profile blocked by the light shielding plate 18 will not immediately change to 0, and the beam profile will be enlarged outward by about 6 // m from the light shielded location. In addition, the edge of the beam profile will be located where the light intensity becomes 20% of the peak chirp. A pulsed laser beam having a pulse energy density distribution of this type is incident on the amorphous silicon film 4 once. A laser beam with a pulse energy density above the threshold 値 that completely melts the amorphous silicon film 4 will melt the irradiated area. When the pulse energy density EL is above the threshold 値, the entire area irradiated by the pulsed laser beam is melted. When the molten part is cooled, crystals grow from the edges of the molten part toward the inside. As shown in Fig. 15A, a large number of crystal grains 100a, which are arranged in the long axis direction of the beam profile, are formed on the side edge behind the moving direction of the incident position of the pulsed laser beam, on the front side edge. A large number of crystalline particles 101a were formed. In the region formed by the region where the crystal grains 100a are formed and the region where the crystal grains 100a are formed, as in the region 8 shown in FIG. 3, microcrystalline grains are formed. The length of crystal growth depends on the temperature of the melting part and the temperature gradient on the solid-liquid interface. The temperature and temperature gradient at the rear side edge are different from the temperature and temperature gradient at the front side edge. Therefore, the lengths of the crystals growing from both sides of the molten region -27-1240957 (24) are different. At the temperature and temperature gradient of the rear side edge, when the conditions for crystal growth are better, the crystal grains 100a formed at the rear side edge are larger than the crystal grains 100a at the front side edge. For example, the horizontal size of crystal grains 100a formed on the rear side edge can reach 7 to 8 // m. Next, the incident position of the pulsed laser beam is moved toward the minor axis of the beam profile, and the pulsed laser beam is incident once. The moving distance of the incident position is set so that the rear side edge of the beam profile of the newly irradiated pulsed laser beam will adjoin or overlap the crystal grain by a distance of 100a. The crystal grains 10a formed on the front side edge during the previous irradiation were melted by this irradiation. As shown in Figure 15B, the rear side edge of the melted area under this irradiation uses crystal grains 100a as seed crystals to grow the crystals in the horizontal direction, forming the size of the inner crystal grains 100a. Crystal grains 100b. When the rear side edge of the beam cross section of the pulsed laser beam radiated this time is adjacent to the crystal grain 100a, the lateral dimension of the crystal grain 100b becomes 14 to 16 &quot; m is about the size of the crystal grain I 0 0 a 2 times. The incident position of the pulsed laser beam is moved in such a manner that the area irradiated by the previous injection and the area irradiated by the current injection partially overlap, and the pulsed laser beam is repeatedly irradiated. The moving distance is set such that the rear side edge of the beam profile of the newly irradiated pulsed laser beam is adjacent to or overlaps with the crystal grains formed on the rear side by the previous irradiation. As shown in Fig. 15C, crystal grains grow in the lateral direction to form large junction crystal grains 100c. At the point in FIG. 15B, the small crystal grains 1 0 1 b that have been formed on the side edge before the beam profile are melted by the subsequent pulsed laser light -28-1240957 (25) and extinguished. In the fifth embodiment, the crystal will grow from the rear side edge of the beam cross section defined by the light shielding plate 18. In the case of the first embodiment, as shown in Fig. 3, the band-shaped region 7 in which large crystal grains are generated is meandering. In the fifth embodiment, since the formation position of the crystal grains 100a is determined artificially by using the light shielding plate 18, the band-shaped region to which the crystal grains 100a are connected is not a meander shape, but a shape almost along a straight line. Therefore, at the time of the second irradiation, the rear side edge of the beam profile can be easily positioned so as to be adjacent to the band-like region where the crystal grains 100a are connected. In addition, the crystal growth direction is uniformly oriented perpendicular to the long axis of the beam profile. In the case where an active device is formed of a polycrystalline film, the direction of the current of the active device formed is parallel to the direction of crystal growth, which can suppress the decrease in carrier mobility caused by the grain boundary. In the above embodiment, each time the pulsed laser beam is incident once, the incident position is moved. In the manner described with reference to FIG. 7, a double pulse is used in which the pulsed laser beam is incident twice in the same position It is also possible to use a multi-pulse method. Thereby, the crystal grains formed can be increased. The preferred area for shading in the skirt part of the pulse energy density distribution shown in Fig. 14 should be a light-shielding area, that is, the pulse energy density Eh and the preferred size of EL can be pluralized by changing the size (wide) of the light-shielding area Obtained through evaluation experiments. The results of the evaluation experiments actually performed are described below. The laser beam emitted from the laser light source will form a long beam with a beam profile with a width of 100 #m 'and a length of 17 mm. The width of the beam profile -29- 1240957 (26) was blocked by light shielding plates on both sides to make a wide 2 2 &quot; m cross-sectional shape, so that the beam profile was imaged on the surface of an amorphous silicon film. The width of the beam profile is half the width of the light intensity distribution. Two laser light sources were used, and the pulse energy densities of the first and second pulsed laser beams on the surface of the amorphous silicon film were set to 550 mJ / cm2 and 500 mj / cm2, respectively, and the delay time was set to 100ns double pulse mode. Under this condition, by irradiating the pulse laser beam twice, the width of the crystal grains 100a formed on the rear side in the scanning direction of the beam profile becomes 3 · 1 // m. Scanning the surface of the non-crystalline silicon film with a pulsed laser beam at a pitch of 3 // m, as shown in Figure 15C, crystals can be continuously grown in the scanning direction. When measuring the orientation of each crystal grain, the <1 1 〇> direction of each crystal grain will be aligned in a direction parallel to the crystal growth direction (scanning direction). Next, a method for manufacturing a polycrystalline film according to the sixth embodiment will be described with reference to FIGS. 16 to 17C. As shown in FIG. 16 'in the sixth embodiment, the part of the skirt portion with the pulse energy density below Eh is shielded by the light shielding plate 18 on the front side of the moving direction of the incident position of the pulsed laser beam, On the rear side, a portion of the skirt portion having a pulse energy density of el or less is shielded by a light shielding plate 18. As shown in Fig. 17A, when one irradiation is performed, larger crystal grains 1 1 0a are formed on the side edge before the beam profile, and smaller crystal grains 1 1 1 a are formed on the rear side edge. As shown in FIG. 17B, when the incident position of the pulsed laser beam is moved and -30- (27) 1240957 is next irradiated, crystal grains 1 1 Ob and 1 1 1 b are formed. Since larger crystal grains Π 〇a are not easily melted ', they will hardly melt after the next irradiation. The crystal grain 1 1 Ob grows from the front edge of the molten region to the rear side (crystal grain 1 10a side). The growth stops when the apex of crystal growth reaches the crystal grains 11. At this time, crystals that use the already formed crystal grains 1 10a as seed crystals and grow in the lateral direction also occur. Therefore, the moving distance of the incident position of the pulsed laser beam can be longer than the width of the crystal grain 1 1. As shown in FIG. 17C, when the incident position of the pulsed laser beam is moved and irradiation is performed repeatedly, large crystal grains 1 1 0a to 1 1 0e are formed. In Fig. 17C, during the third irradiation, smaller crystal grains 1 1 1 c are formed on the side edges after the beam profile. In the fourth and subsequent irradiations, since the lateral side edges of the beam profile are located inside the larger crystal grains 1 10a to 1 10e, no melting portion occurs near the rear side edges. In the sixth embodiment, as shown in FIG. 17C, for example, a clear boundary is formed between the band-shaped region where the crystal grains 110a are connected and the band-shaped region where the crystal grains 110b are connected. The position of this boundary is determined by 18 people by the shading plate. For example, when an active device is formed by a polycrystalline silicon thin film, the boundary of the crystalline particles may be arranged so that the active device does not cross the boundary of the crystalline particles. As described above, the entire substrate can be covered with a band-shaped area as shown in FIG. 9. The results of the evaluation experiments actually performed are described below. The laser beam emitted from the laser light source will form a long beam with a beam width of 100 // m and a beam length of -31-1240957 (28) 17 mm. The scanning direction of the beam profile is shielded by a light shielding plate at the front side edge to form a wide cross section of 5 μm, so that the beam profile is imaged on the surface of the amorphous silicon film. Using two laser light sources, and setting the pulse energy densities of the first and second pulsed laser beams on the surface of the amorphous silicon film to 710 mJ / cm2 and 640 mJ / cm2, respectively, The delay time is set to a double pulse mode of 200 ns. Under this condition, by irradiating the pulsed laser beam twice, the width of the crystal grains 1 0 0 a formed on the front side in the scanning direction of the beam profile becomes 5 · 4 m. Scanning the surface of the non-crystalline silicon film with a pulsed laser beam at a pitch of 1 2 // m can form a 12 m wide band-shaped region connected by crystal grains in the long side of the beam profile. The crystal grains of adjacent band-shaped regions will contact each other at the boundaries of the band-shaped regions, and they will be fully polycrystalline. Regardless of whether the width of the crystal grains 1 l0a formed under one irradiation is 5. 4 m, the width of the final band-shaped area will become 1 2 // m, which is a width of 5 formed by one irradiation. 4 // m crystal grains are used as seed crystals, and the subsequent irradiation will cause crystal growth in the horizontal direction. This growth process is the same as the crystal growth process described in FIGS. 8A to 8G. In the above-mentioned evaluation experiments of the fifth and sixth examples, a double pulse method was used. At this time, the delay time from the first pulse laser beam to the second pulse laser beam is preferably set to 100 to 100 ns. The appropriate delay time is slightly shorter than the delay time in the case where no shading plate is used. This is because the slope of the light intensity distribution on both sides of the beam profile is steep, and the curing speed is faster than in the case where no light shielding plate is used. Next, a seventh embodiment will be described. In the fifth and sixth embodiments -32- 1240957 (29), the lateral width direction of the beam profile is such that the light intensity distribution (or pulse energy density distribution) forms an asymmetric manner, and The light-shielding plate shields light, but it may shield light in a symmetrical manner. If the light intensity distribution becomes symmetrical, crystal particles of almost the same size will be formed on the side edges and the rear side edges in the scanning direction. Therefore, the second embodiment described with reference to Figs. 8A to 8G, and the third embodiment described with reference to Figs. 12A and 12B, or Figs. 13A and 13B The same method as described in the fourth embodiment can be used to perform polycrystallization of an amorphous silicon film. In the above fifth to seventh embodiments, the light beam cross section at the position where the light shielding plate is arranged is imaged on the surface of the amorphous silicon film, but the light shielding plate may be arranged close to the amorphous silicon film. The distance between the light-shielding plate and the amorphous silicon film can be, for example, 0.  About 1 mm. In the above-mentioned first and sixth embodiments, a part of the laser beam is shielded by a light-shielding plate to form a laser beam having an asymmetric light intensity distribution in a broad direction of the beam profile. However, other optical devices are used to separate the light. The intensity distribution may be made asymmetric. For example, a gradient filter in which a dot pattern of chromium (C0, etc.) is disposed on the surface of the quartz glass may be disposed in the optical path. The present invention will be described in accordance with the above embodiments, but the present invention is not limited to this. Various possible changes, improvements, combinations, etc. [Schematic description] Figure 1 is a schematic plan view of a laser annealing device used in the embodiment -33-1240957 (30) Figure 2A is a cross-section of a processing object Fig. 2 is a diagram showing the pulse energy density distribution of the pulsed laser beam on the surface of the object to be processed in the first embodiment, and Fig. 2B is a schematic plan view of the polycrystallized object to be processed. A SEM photograph of a polycrystalline film produced in accordance with the method of the first embodiment is depicted. Figure 4A is a graph showing the relationship between the temperature of the molten silicon and the crystal growth rate, and Figure 4B is a graph showing the relationship between the temperature and the nucleation rate. Figure 5 A shows the relationship between the width of the beam profile and the size of the crystal grains. Figure 5 B shows the relationship between the gradient of the pulse energy density distribution and the size of the crystal grains. Figure 6 shows the pulse width Figure 7 shows the relationship between the crystal grain size. Figure 7 shows an example of the laser beam waveform when a pulsed laser beam is irradiated twice at one place. Figure 8 is a schematic diagram showing as many as in the second embodiment. The cross-section of the thin film during the manufacturing process of the crystal film manufacturing method. Figure 9 is a SEM photograph depicting the polycrystalline film manufactured according to the method of the second embodiment. Figure 10 shows the length of crystal growth per irradiation Figure 1 shows the relationship between the overlap ratio necessary for full polycrystallization. Figure 1 1 shows the wavelength dependence of the absorption coefficient of single crystalline silicon and amorphous silicon. Figure 1 2 A shows the implementation in accordance with the third Example of the production of polycrystalline film-34- (31) 1240957 The relationship between the pulse energy density distribution of the pulsed laser beam and the polycrystalline region, Figure 1 2B shows the pattern of the polycrystalline film being manufactured. Plan view. Figure 1 3A is a diagram showing the relationship between the pulse energy density distribution of a pulsed laser beam and a polycrystalline region used in the method for manufacturing a polycrystalline film according to the fourth embodiment, and Figure 1 3B is a Mode of manufacturing polycrystalline film Figures 14 and 14 are cross-sectional views of the substrate to be processed and the light-shielding plate and the distribution of pulse energy density according to the method for manufacturing a polycrystalline film according to the fifth embodiment. Figures 15A to 15C are used to show A schematic diagram of polycrystallization according to the method for manufacturing a polycrystalline film according to the fifth embodiment. Figure 16 is a sectional view showing a substrate to be processed and a light-shielding plate used in the method for manufacturing a polycrystalline film according to the sixth embodiment. And the distribution of the pulse energy density. Figures 17 A to 17 C are schematic diagrams showing polycrystallization in accordance with the method for manufacturing a polycrystalline film according to the sixth embodiment. Figure No. 40 processing chamber 44 platform 6 〇 Sliding mechanism 6 3, 6 5 Combined member 64 Linear guide mechanism-35- 1240957 66 (32) Linear motor 67 Telescopic hose 7 1 Laser light source 72 Homogenizer 82 Transfer chamber 83.  84 Moving in and out of the room 85, 86, 87 Gate valve 88 C C D Camera 89 Video monitor 94 Moving robot arm -36-

Claims (1)

(1) 1240957 拾、申請專利範圍 1 · 一種多結晶膜之製造方法，其特徵爲具有： (a )準備在表面上形成由非結晶質材料構成之薄膜 之加工對象物的工程，及 (b)在前述薄膜表面使在一方向具有較長光束剖面 之脈衝雷射光束朝該薄膜射入，使該薄膜溶融後固化，在 光束射入區域的長軸方向延伸之邊緣與中心線之間的區域 之中，自該邊緣以及該中心線起僅被隔開某段距離的延伸 於該長軸方向之第1帶狀區域內，產生在該長軸方向上連 接之結晶粒之工程。 2 .如申請專利範圍第1項之多結晶膜之製造方法，其 中前述工程（b)之後進而具有 (c )脈衝雷射光束的射入位置朝光束射入區域的短 軸方向移動，不使在前述第1帶狀區域內所產生的結晶粒 完全溶融，以鄰接於該結晶粒之區域的前述薄膜溶融之條 件下使脈衝雷射光束射入，將該結晶粒作爲種晶’在則述 帶狀區域之兩側使結晶生長之工程。 3 ·如申請專利範圍第2項之多結晶膜之製造方法，其 中 則述工程（c )方面，脈衝雷射光束之射入區域的移 動方向前方側緣與中心線之間的區域中，自該側緣起僅被 隔開某段距離，且自前述第1帶狀區域起亦僅被隔開某段 距離，延伸於長軸方向之第2帶狀區域內，產生在該長軸 方向上連接之結晶粒，前述工程（c )之後，進而具有 -37- (2) 1240957 (d )使脈衝雷射光束之射入位置朝短軸 同時使脈衝雷射光束射入前述薄膜，使自前述 域向前述第2帶狀區域生長之結晶粒，與自前 區域向前述第1帶狀區域生長之結晶粒接觸之 4 .如申請專利範圍第1項之多結晶膜之製 中前述工程（b)之後，進而具有 (e )脈衝雷射光束之射入位置朝光束射 軸方向移動，且不使前述第1帶狀區域內所產 溶融，被挾在前述第1帶狀區域的區域的前述 接著位於光束射入區域之移動方向之前方側的 域之前方側緣的區域的前述薄膜，在溶融條件 射光束射入，且在溶融之區域產生結晶粒之工 該工程（e)方面，在被挾在前述第1帶 域內所產生之結晶粒，會接觸到產生於其兩側 區域內的結晶粒，而產生於光束射入區域之移 方側的第1帶狀區域之前方側的結晶粒，則以 1帶狀區域內所產生中的結晶粒的條件下使脈 射入。 5 .如申請專利範圍第1項之多結晶膜之製 中前述工程（b)之後，進而具有 (e )脈衝雷射光束之射入位置朝光束射 軸方向移動，且不使前述第1帶狀區域內所產 溶融，被挾在前述第1帶狀區域的區域的前述 接著位於光束射入區域之移動方向之前方側的 方向移動， 第1帶狀區 述第2帶狀 工程。 丨造方法，其 入區域之短 生之結晶粒 薄膜，以及 第1帶狀區 下使脈衝雷 程， 狀區域之區 之第1帶狀 動方向之前 接觸到該第 衝雷射光束 造方法，其 入區域之短 生之結晶粒 薄膜，以及 第1帶狀區 -38- 1240957 (3) 域之前方側緣的區域的前述薄膜，在溶融條件下使脈衝雷 射光束射入，於被挾在前述第1帶狀區域之溶融區域內’ 將兩側之前述第1帶狀區域內之結晶粒作爲種晶使結晶生 長，使這些自兩側生長之結晶粒接觸，在位於光束射入區 域之移動方向之前方側的第1帶狀區域之前方側的溶融區 域，將該第1帶狀區域內之結晶粒作爲種晶使結晶生長。 6. 如申請專利範圍第1項之多結晶膜之製造方法，其 中 前述前述薄膜係由矽所形成，射入該薄膜之脈衝雷射 光束之波長則爲340〜900nm。 7. 如申請專利範圍第1項之多結晶膜之製造方法，其 中 前述工程（b )方面，使脈衝雷射光束射入1次後， 在溶融之部分完全固化前，朝相同位置射入第2次。 8 .如申請專利範圍第1項之多結晶膜之製造方法，其 中 在前述工程（b )被照射之脈衝雷射光束之脈衝能量 密度之短軸方向的梯度，於前述第1帶狀區域之長軸方向 所延伸之外側緣，爲280mJ/ cm2/ # m以下。 9·如申請專利範圍第8項之多結晶膜之製造方法，其 中 在前述工程（b )被照射之脈衝雷射光束之脈衝能量 密度之短軸方向的梯度，於前述第1帶狀區域之長軸方向 所延伸之外側緣，爲1 0 m J / c m2 / y m以上。 -39- (4) 1240957 1 0 ·如申請專利範圍第1項之多結晶膜之製造方法， 其中 前述工程（b )方面，鄰接前述第1帶狀區域，而比 該第1帶狀區域更外側之一部份區域，被形成小於該第1 帶狀區域內之結晶粒之結晶粒隨機（random )分佈而形成 隨機分佈區域，且照射脈衝雷射光束，其脈衝能量密度分 佈使自該隨機分佈區域與非結晶區域之邊界，至前述第1 帶狀區域爲止的間隔成爲1 5 // m以上。 1 1 . 一種多結晶膜之製造方法，其特徵爲具有： (i )準備在表面上形成由非結晶質材料構成之薄膜 之加工對象物的工程，及 (j)在前述薄膜之表面使在一方向具有長光束剖面 之脈衝雷射光束朝該薄膜射入，使該薄膜溶融後固化使多 結晶化之工程，在以自光束射入區域之長軸方向所延伸之 邊緣向內側僅被隔開某段距離的假想線，與以該光束射入 區域之中心線被劃定之第I帶狀區域內，產生在該長軸方 向上連接之結晶粒，而使前述中心線之一方之側的前述第 1帶狀區域內所產生之結晶粒，與另一方之第1帶狀區域 內所產生之結晶粒相互接觸的條件下使脈衝雷射光束射入 之工程； 脈衝雷射光束之脈衝能量密度的短軸方向的梯度，於 前述第1帶狀區域的長軸方向所延伸的外側緣，爲2 8 OmJ /cm2/ //m 以下。 i 2 .如申請專利範圍第1 1項之多結晶膜之製造方法， -40- 1240957 (5) 其中 前述脈衝雷射光束之脈衝能量密度的短軸方向的梯度 ，於前述第〗帶狀區域的長軸方向所延伸的外側緣，爲 10mJ / cm2/ &quot;m 以上。 1 3 ·如申請專利範圍第1 1項之多結晶膜之製造方法’ 其中 前述工程（j )方面，使脈衝雷射光束射入1次後’ 在溶融之部分完全固化前射入第2次。 1 4 ·如申請專利範圍第1 1項之多結晶膜之製造方法， 其中前述工程（j)之後進而具有 (k )使脈衝雷射光束之射入位置朝光束射入區域之 短軸方向移動，同時一次次使脈衝雷射光束射入該薄膜， 使該薄膜溶融後固化使多結晶化之工程， 執行1次用以溶融與固化之脈衝雷射光束照射之條件 爲：在以自光束射入區域之長軸方向所延伸之邊緣向內側 僅被隔開某段距離之假想線，與以該光束射入區域之中心 線被劃定之第2帶狀區域內，產生在該長軸方向上連接之 結晶粒，而在前述中心線之一方之側之前述第2帶狀區域 內所產生之結晶粒，與在另一方之第2帶狀區域內所產生 之結晶粒會相互接觸，且在移動方向之後方側之第2帶狀 區域內所產生之結晶粒，會接觸到在移動方向之後方側已 被形成之結晶粒。 1 5 .如申請專利範圍第11項之多結晶膜之製造方法， 其中 -41 - (6) 1240957 前述薄膜係由矽所形成，射入該薄膜之脈衝雷射光束 之波長則爲340〜900nm。 1 6 ·如申請專利範圍第1 1項之多結晶膜之製造方法， 其中 前述工程（j)方面，在鄰接前述第1帶狀區域，而 比該桌1帶狀區域更外側之一部份區域，被形成小於該第 1帶狀區域內之結晶粒之結晶粒隨機分佈而形成隨機分佈 區域，且照射脈衝雷射光束，其脈衝能量密度分佈使自該 隨機分佈區域與非結晶區域之邊界，至前述第1帶狀區域 爲止的間隔成爲1 5 e m以上。 1 7. —種多結晶膜之製造方法，其特徵爲具有： (p )準備在表面上形成由非結晶質材料構成之薄膜 之加工對象物的工程，及 (q)在前述薄膜之表面使在一方向具有長光束剖面 之脈衝雷射光束朝該薄膜射入，使該薄膜溶融後固化使多 結晶化之工程，其中脈衝雷射光束之射入工程之光束密度 分佈（profile )方面，即脈衝雷射光束之脈衝能量密度之 短軸方向的梯度’於已溶融區域之邊緣爲280mJ/cm2/ m以下。 1 8 .如申請專利範圍第1 7項之多結晶膜之製造方法， 其中 前述工程（q )方面，被射入之脈衝雷射光束之脈衝 能量密度之短軸方向的梯度’於已溶融區域之邊緣爲 以上。 -42- (7) 1240957 1 9 .如申請專利範圍第1 7項之多結晶膜之製造方法， 其中 前述薄膜係由矽所形成，射入該薄膜之脈衝雷射光束 之波長則爲3 4 0〜9 0 0 n m。 20.如申請專利範圍第1 7項之多結晶膜之製造方法， 其中 前述工程（q )方面，使脈衝雷射光束射入1次後， 在溶融之部分完全固化前，朝相同位置射入第2次。 2 1 ·如申請專利範圍第1 7項之多結晶膜之製造方法， 其中 前述工程（q)方面，鄰接前述第1帶狀區域，而比 該第1帶狀區域更外側之一部份區域，被形成小於該第1 帶狀區域內之結晶粒之結晶粒隨機分佈而形成隨機分佈區 域，且照射脈衝雷射光束，其脈衝能量密度分佈使自該隨 機分佈區域與非結晶區域之邊界，至前述第1帶狀區域爲 止的間隔成爲1 5 // m以上。 2 2 . —種在下底基板之表面上形成由多結晶材料構成 之多結晶膜，其特徵爲： 各自包含連接在基板面內之第1方向之由複數之結晶 粒所形成的複數之結晶粒列。 2 3 .如申請專利範圍第2 2項之多結晶膜，其中 前述結晶粒列係配列於與前述第1方向垂直之第2方 向，該結晶粒列內之結晶粒則接觸到鄰接之結晶粒列內之 結晶粒。 -43- 1240957 (8) 2 4 .如申請專利範圍第2 2項之多結晶膜，其中 前述結晶粒列之寬幅係固定。 2 5 .如申請專利範圍第2 2項之多結晶膜，其中 前述結晶粒列係複數個被配置於與前述第1方向垂直 之第2方向’於前述第2方向之各結晶粒列內之結晶粒的 平均大小爲1 · 5 // m以上。 2 6 .如申請專利範圍第2 2項之多結晶膜，其中 於則述弟1方向之則述結晶粒列內之結晶粒的平:均大 小爲〇 . 7 # ni以上。 2 7 .如申請專利範圍第2 2項之多結晶膜，其中 在接著前述結晶粒列之一方之邊緣的區域，結晶粒小 於該結晶粒列內之結晶粒會隨機分佈形成隨機分佈區域， 該隨機分佈區域之寬幅爲1 5 μ m以上。 2 8 . —種多結晶膜之製造方法，其特徵爲具有： (a )準備在表面上形成由非結晶質材料構成之薄膜 之加工對象物的工程，及 (b) 在前述薄膜之表面使在一方向具有長光束剖面 的脈衝雷射光束朝該薄膜射入至少1回之工程，關於該光 束剖面之短軸方向的光強度分佈方面，係形成中央部大而 愈靠近邊緣愈小，爲非對稱之第1形狀，及 (c) 脈衝雷射光束之射入位置，在前述薄膜之表面 上，會朝與該脈衝雷射光束之光束剖面的長軸方向垂直的 方向移動，而且以部分重疊前次被照射之區域的方式，使 脈衝雷射光束之射入位置與前述加工對象物之至少一方移 -44- 1240957 (9) 動之工程，及 (d )使光強度分佈具有前述第1形狀的脈衝雷射光 束朝前述薄膜至少射入1回之工程，及 (e )輪流反覆進行前述工程（c )與工程（d )之工 程。 2 9 ·如申請專利範圍第2 8項之多結晶膜之製造方法， 其中 前述工程（b)方面，藉由在關於光束剖面之短軸方 向的光強度分佈具有中央部大而愈靠近邊緣愈小之形狀的 分佈之中，一方之第1裙襬部之第1光強度以下的部分被 遮罩遮光，另一方之第2裙襬部的部分未被遮光，或者該 第2裙襬部之低於該第1光強度之第2光強度以下的部分 被遮光，而獲得前述脈衝雷射光束。 3 0.如申請專利範圍第29項之多結晶膜之製造方法， 其中 前述工程（b )方面，從光束剖面之前述第1裙襬部 側緣向內側僅使結晶生長某段長度，形成在光束剖面之長 邊方向連接的複數結晶粒， 前述工程（c )方面，以使光束剖面之前述第2裙襬 部側成爲移動方向之前方的方式，使脈衝雷射光束之射入 位置在前述薄膜上進行相對地移動，該移動距離爲’在前 次照射下從光束剖面之前述第1裙襬部側緣開始生長的結 晶粒，鄰接或者重疊光束剖面之第1裙襬部側緣的距離， 前述工程（d )方面，以前次照射下已生長之結晶粒 -45- 1240957 do) 作爲種晶，從該種晶向光束剖面之內側使結晶生長t 3 1 .如申請專利範圍第2 9項之多結晶膜之製造方法， 其中 前述工程（b )方面，從光束剖面之前述第1裙襬部 側緣向內側僅使結晶生長某段長度，形成在光束剖面之長 邊方向連接的複數結晶粒， 前述工程（c )方面，以使光束剖面之前述第1裙襬 部側成爲移動方向之前方的方式，使脈衝雷射光束之射入 位置在前述薄膜上進行相對地移動， 前述工程（d )中被照射之脈衝雷射光束之在前述薄 膜表面的脈衝能量密度，係前次爲止之照射下在前述第1 裙襬部側被形成之結晶粒不會再溶融的大小，從光束剖面 之前述第1裙襬部側緣向內側僅使結晶生長某段長度，形 成在光束剖面之長邊方向連接的複數結晶粒。 3 2 .如申請專利範圍第3 1項之多結晶膜之製造方法， 其中 前述工程（c )方面，脈衝雷射光束之射入位置之移 動距離，係前述工程（d )中生長之結晶粒鄰接到前次照 射下被形成之結晶粒的距離。 3 3 .如申請專利範圍第2 8項之多結晶膜之製造方法， 其中 前述薄膜係由矽所形成，射入該薄膜之脈衝雷射光束 的波長爲340〜900nm。 3 4.—種多結晶膜之製造方法，其特徵爲具有： • 46 - 1240957 (11) (a )準備在表面上形成由非結晶質材料構成之薄 之加工對象物的工程，及 (b) 在前述薄膜之表面使在一方向具有長光束剖 的脈衝雷射光束朝該薄膜射入至少1回之工程，關於該 束剖面之短軸方向的光強度分佈，係在具有中央部大而 罪近邊緣愈小的形狀的分佈之中’至少〜方之第1裙辛罷 的部分會被遮罩遮光的第1形狀，及 (c) 脈衝雷射光束之射入位置，在前述薄膜之表 上，會朝與該脈衝雷射光束之光束剖面的長軸方向垂直 方向移動，而且以部分重疊前次被照射之區域的方式， 脈衝雷射光束之射入位置與前述加工對象物之至少一方 動之工程，及 (d )使光強度分佈具有前述第1形狀的脈衝雷射 束朝前述薄膜至少射入1回之工程，及 (e )輪流反覆進行前述工程（c )與工程（d )之 程。 3 5 · —種多結晶膜之製造方法，其特徵爲具有： (a )準備在表面上形成由非結晶質材料構成之薄 之加工對象物的工程，及 (b)在前述薄膜之表面使在一方向具有長光束剖 的脈衝雷射光束朝該薄膜射入，使該薄膜溶融後固化， 光束射入區域的長軸方向延伸之邊緣與中心線之間的區 之中，自該邊緣以及該中心線起僅被隔開某段距離的延 於該長軸方向之第1帶狀區域內產生結晶粒，在鄰接前 膜 面 光 愈 部 面 的 使 移 光 工 膜 面 在 域 伸 述 -47- (12) 1240957 第1帶狀區域，而比該第1帶狀區域再外側之一部的區域 ，結晶粒小於被形成於該第1帶狀區域內之結晶粒會隨機 分佈形成隨機分佈區域的工程。(1) 1240957, patent application scope 1 · A method for manufacturing a polycrystalline film, comprising: (a) a process of preparing a processing object to form a thin film made of an amorphous material on a surface, and (b ) A pulsed laser beam with a longer beam profile in one direction is incident on the film surface, and the film is melted and solidified after melting. The distance between the edge extending in the direction of the long axis of the beam incident area and the center line In the area, a process of generating crystal grains connected in the long axis direction in the first strip-shaped area extending in the long axis direction by a certain distance from the edge and the center line is separated. 2. The method for manufacturing a polycrystalline film according to item 1 of the scope of the patent application, wherein after the aforementioned step (b) and then (c), the incident position of the pulsed laser beam is moved toward the short axis direction of the incident region of the beam without causing The crystal grains generated in the first band-shaped region are completely melted, and a pulsed laser beam is incident under the condition that the thin film adjacent to the crystal grains is melted, and the crystal grains are used as seed crystals. The process of growing crystals on both sides of the banded area. 3. If the method for manufacturing a polycrystalline film according to item 2 of the scope of patent application, in the aspect (c), the area between the front edge and the center line of the moving direction of the impinging area of the pulsed laser beam, since The side edge is only separated by a certain distance, and it is also separated by a certain distance from the first strip-shaped area. It extends in the second strip-shaped area in the long-axis direction, resulting in a connection in the long-axis direction. The crystal grains, after the aforementioned process (c), further have -37- (2) 1240957 (d) so that the incident position of the pulsed laser beam is directed toward the short axis while the pulsed laser beam is incident on the film, so that The crystal grains growing to the second band-shaped region are in contact with the crystal grains growing from the front region to the first band-shaped region. 4. After the aforementioned process (b) in the production of the polycrystalline film in the first patent application scope And further has (e) the incident position of the pulsed laser beam moving in the direction of the beam axis without dissolving the products produced in the first band-shaped region, and being located next to the region of the first band-shaped region. The direction of the beam's incident area In the process (e) of the thin film in the area in front of the side of the square side, the beam is irradiated under the melting conditions, and crystal grains are generated in the molten area. The generated crystal grains will contact the crystal grains generated in the areas on both sides thereof, and the crystal grains generated on the front side of the first band-shaped region on the shift side of the beam incident region will be in a band-shaped region. Pulses are injected under the conditions of the generated crystal grains. 5. After the above-mentioned project (b) in the production of the polycrystalline film in item 1 of the scope of the patent application, the position of the (e) pulsed laser beam is moved toward the beam axis without the first band. The melt produced in the band-shaped region is moved in the direction of the first band-shaped region, which is located next to the moving direction of the beam incident region, and the first band-shaped region describes the second band-shaped process.丨 manufacturing method, the short-lived crystalline grain film entering the area, and the first band-shaped region to make the pulsed laser range, the first band-shaped region of the region-shaped area before the first laser beam contact method, The short-lived crystalline grain film entering the region, and the aforementioned film in the region on the side of the front side of the first band-38-1240957 (3) region, the pulsed laser beam is incident under the melting conditions, and In the melting zone of the aforementioned first band-shaped region, the crystal grains in the aforementioned first band-shaped region on both sides are used as seed crystals to grow crystals, and the crystal grains grown from the two sides are brought into contact with each other in the beam-entering region. In the molten zone on the front side of the first band-shaped region on the front side of the moving direction, crystal grains in the first band-shaped region are used as seed crystals to grow crystals. 6. The method for manufacturing a polycrystalline film according to item 1 of the application, wherein the aforementioned thin film is formed of silicon, and the wavelength of a pulsed laser beam incident on the thin film is 340 to 900 nm. 7. The method for manufacturing a polycrystalline film according to item 1 of the scope of the patent application, wherein in the above-mentioned process (b), after the pulsed laser beam is injected once, before the melted part is completely solidified, the first part is injected into the same position. 2 times. 8. The method for manufacturing a polycrystalline film according to item 1 of the scope of patent application, wherein the gradient in the minor axis direction of the pulse energy density of the pulsed laser beam irradiated in the aforementioned process (b) is in the first band-shaped region. The outer side edge extended in the long axis direction is 280mJ / cm2 / # m or less. 9. The method for manufacturing a polycrystalline film according to item 8 of the scope of the patent application, wherein the gradient in the minor axis direction of the pulse energy density of the pulsed laser beam irradiated in the aforementioned process (b) is in the first band-shaped region. The outer side edge extending in the long axis direction is 10 m J / c m2 / ym or more. -39- (4) 1240957 1 0 · For the method for manufacturing a polycrystalline film according to item 1 of the scope of patent application, in the aspect (b), the first band-shaped region is adjacent to the first band-shaped region and is more than the first band-shaped region. A part of the outer area is formed by a random distribution of crystal grains smaller than the crystal grains in the first band-shaped region to form a random distribution region, and a pulsed laser beam is irradiated, and its pulse energy density distribution is The boundary between the distribution region and the amorphous region, and the interval between the first band-shaped region and the first band-shaped region is 1 5 // m or more. 1 1. A method for manufacturing a polycrystalline film, comprising: (i) a process of preparing a processing object to form a thin film made of an amorphous material on a surface, and (j) forming a thin film on the surface of the thin film. A pulsed laser beam with a long beam profile in one direction is incident on the film, and the film is melted and solidified to make the polycrystallize. The edge extending from the direction of the long axis of the beam incident area is only separated from the inside. Open an imaginary line of a certain distance, and in the first band-shaped area demarcated by the center line of the area where the light beam is incident, crystal grains connected in the long axis direction are generated, so that one side of the aforementioned center line The process of making a pulsed laser beam enter the crystal grains generated in the aforementioned first band-shaped region and the crystal grains generated in the other first band-shaped region in contact with each other; The gradient in the minor axis direction of the energy density is 2 8 OmJ / cm2 / // m or less at the outer edge extending in the major axis direction of the first strip-shaped region. i 2. The method for manufacturing a polycrystalline film according to item 11 of the scope of patent application, -40-1240957 (5) where the gradient of the short-axis direction of the pulse energy density of the aforementioned pulsed laser beam is in the aforementioned zone The outer edge extending in the direction of the long axis is 10mJ / cm2 / &quot; m or more. 1 3 · The method for manufacturing a polycrystalline film according to item 11 of the scope of the patent application, where the aforementioned process (j), after the pulsed laser beam is injected once, is injected for the second time before the melted part is completely cured. . 1 4 · The method for manufacturing a polycrystalline film according to item 11 of the scope of patent application, wherein after the aforementioned process (j), there is (k) to move the incident position of the pulsed laser beam toward the short axis direction of the incident region of the beam At the same time, the pulse laser beam is incident into the film again and again, and the film is melted and solidified to make the crystallize. The conditions for performing the pulse laser beam irradiation for melting and curing once are: The edge extending in the direction of the long axis of the entrance area is separated from the imaginary line only a certain distance inward, and the second strip-shaped area demarcated by the center line of the incident area of the light beam is generated in the direction of the long axis The crystal grains connected to each other, and the crystal grains generated in the second band-shaped region on one side of the center line and the crystal grains generated in the second band-shaped region on the other side will contact each other, and The crystal grains generated in the second band-shaped area on the side after the moving direction will contact the crystal grains that have been formed on the side after the moving direction. 15. The method for manufacturing a polycrystalline film according to item 11 of the scope of patent application, in which -41-(6) 1240957 the aforementioned thin film is formed of silicon, and the wavelength of the pulsed laser beam incident on the thin film is 340 to 900 nm . 16 · The method for manufacturing a polycrystalline film according to item 11 of the scope of the patent application, wherein in the aforementioned process (j), the part adjacent to the first band-shaped region and further outside than the band-shaped region of the table 1 A random distribution area is formed by crystalline particles smaller than the crystalline particles in the first band-shaped area, and a pulsed laser beam is irradiated, and its pulse energy density distribution is from the boundary between the random distribution area and the amorphous area. The interval to the first band-shaped region is 15 em or more. 1 7. A method for manufacturing a polycrystalline film, comprising: (p) a process of preparing a processing object to form a thin film made of an amorphous material on a surface, and (q) forming a surface of the thin film A pulsed laser beam having a long beam profile in one direction is incident on the film, and the film is melted and solidified to cause polycrystallization. The pulse density of the laser beam is projected in terms of the profile of the beam, The gradient in the minor axis direction of the pulse energy density of the pulsed laser beam is 280 mJ / cm2 / m or less at the edge of the melted area. 18. The method for manufacturing a polycrystalline film according to item 17 in the scope of the patent application, wherein in the aforementioned process (q), the gradient of the short-axis direction of the pulse energy density of the incident pulse laser beam is in the molten region The edges are above. -42- (7) 1240957 1 9. The method for manufacturing a polycrystalline film according to item 17 of the scope of patent application, wherein the thin film is made of silicon, and the wavelength of the pulsed laser beam incident on the thin film is 3 4 0 to 9 0 0 nm. 20. The method for manufacturing a polycrystalline film according to item 17 in the scope of the patent application, wherein in the aforementioned process (q), after the pulsed laser beam is injected once, before the molten part is completely cured, it is injected into the same position. 2nd. 2 1 · The method for manufacturing a polycrystalline film according to item 17 in the scope of the patent application, wherein in the aspect (q) of the aforementioned process, it is adjacent to the first band-shaped region, and is a part of an area outside the first band-shaped region. The random distribution area is formed by the random distribution of crystalline particles smaller than the crystalline particles in the first band-shaped area, and the pulsed laser beam is irradiated with a pulse energy density distribution from the boundary between the random distribution area and the amorphous area. The interval to the first band-shaped region is 1 5 // m or more. 2 2. — A polycrystalline film made of a polycrystalline material is formed on the surface of the lower substrate, and each of the polycrystalline films includes a plurality of crystal grains formed by a plurality of crystal grains connected in a first direction in the substrate surface. Column. 2 3. The polycrystalline film according to item 22 of the scope of patent application, wherein the crystal grain rows are arranged in a second direction perpendicular to the first direction, and the crystal grains in the crystal grain rows contact adjacent crystal grains. Crystal grains in the column. -43- 1240957 (8) 2 4. The polycrystalline film according to item 22 of the patent application scope, wherein the width of the aforementioned crystal grain row is fixed. 2 5. The polycrystalline film according to item 22 of the scope of the patent application, wherein the crystal grain rows are arranged in a plurality of crystal grain rows in a second direction perpendicular to the first direction and in the crystal grain rows in the second direction. The average size of crystal grains is 1 · 5 // m or more. 26. The polycrystalline film according to item 22 of the scope of patent application, wherein the flatness of the crystal grains in the crystal grain row in the direction of Zesi 1 is equal to or greater than 0.7 # ni. 27. The polycrystalline film according to item 22 of the scope of patent application, wherein in the area following the edge of one of the aforementioned crystal grain rows, the crystal grains smaller than the crystal grains in the crystal grain row will be randomly distributed to form a random distribution region. The width of the randomly distributed area is more than 15 μm. 2 8. A method for manufacturing a polycrystalline film, comprising: (a) a process of preparing a processing object to form a thin film made of an amorphous material on a surface, and (b) using a surface of the thin film For a project in which a pulsed laser beam with a long beam profile is incident on the film at least once in one direction, regarding the light intensity distribution in the short axis direction of the beam profile, the central part is formed to be larger and the closer to the edge, the smaller the The asymmetric first shape and (c) the incident position of the pulsed laser beam will move on the surface of the film in a direction perpendicular to the long axis direction of the beam profile of the pulsed laser beam, and partly The method of overlapping the previously irradiated area moves the incident position of the pulsed laser beam and at least one of the aforementioned processing objects by -44-1240957 (9) moving the project, and (d) making the light intensity distribution A project in which a pulse laser beam of a shape is incident at least once toward the aforementioned film, and (e) the aforementioned projects (c) and (d) are carried out repeatedly in turn. 2 9 · The method for manufacturing a polycrystalline film according to item 28 of the scope of patent application, wherein in the aforementioned process (b), the light intensity distribution in the short-axis direction with respect to the beam profile has a large central portion, and the closer to the edge, the more In the distribution of small shapes, the part below the first light intensity of the first skirt part of one side is blocked by a mask, and the part of the second skirt part of the other side is not blocked, or the part of the second skirt part is not blocked. The portion lower than the second light intensity of the first light intensity is shielded from light, and the aforementioned pulsed laser beam is obtained. 30. The method for manufacturing a polycrystalline film according to item 29 of the scope of the patent application, wherein in the aforementioned process (b), only a certain length of crystal is grown from the side edge of the first skirt portion to the inner side of the beam profile, and is formed in For the plurality of crystal grains connected in the longitudinal direction of the beam profile, in the step (c), the incident position of the pulsed laser beam is set so that the second skirt portion side of the beam profile is in front of the moving direction. The film is relatively moved, and the moving distance is' the distance between the crystal grains growing from the side edge of the first skirt portion of the beam profile under the previous irradiation and the side edge of the first skirt portion which is adjacent to or overlaps the beam profile. In the aspect of the aforementioned project (d), the crystal grain -45-1240957 do) which has grown under the previous irradiation is used as a seed crystal, and the crystal is grown from the seed crystal to the inside of the beam profile t 3 1. The method for manufacturing a polycrystalline film according to the item, wherein in the aspect (b), the crystal is grown only a certain length from the side edge of the first skirt portion inward to the beam profile, and is formed on the long side of the beam profile. With respect to the connected plurality of crystal grains, in the step (c), the incident position of the pulsed laser beam is relatively opposed to the film so that the first skirt portion side of the beam cross section becomes forward of the moving direction. Movement, the pulse energy density of the pulsed laser beam irradiated in the aforementioned process (d) on the surface of the film is the crystal grains formed on the side of the first skirt portion under the previous irradiation will not be melted again The size is such that the crystal grows only a certain length from the side edge of the first skirt portion inward from the beam profile to form a plurality of crystal grains connected in the longitudinal direction of the beam profile. 32. The method for manufacturing a polycrystalline film according to item 31 of the scope of the patent application, wherein in the aforementioned process (c), the moving distance of the incident position of the pulsed laser beam is the crystal grains grown in the aforementioned process (d) The distance adjacent to the crystal grains formed under the previous irradiation. 33. The method for manufacturing a polycrystalline film according to item 28 of the patent application range, wherein the thin film is formed of silicon, and the wavelength of the pulsed laser beam incident on the thin film is 340 to 900 nm. 3 4. A method for manufacturing a polycrystalline film, which is characterized by: • 46-1240957 (11) (a) a process of preparing a thin processing object made of an amorphous material on a surface, and (b ) A process in which a pulsed laser beam having a long beam cross section in one direction is incident on the film at least once toward the film. The light intensity distribution in the short axis direction of the beam cross section is large and has a central portion. Among the distribution of smaller shapes near the edge of sin, at least the first shape of Fang's first skirt will be shielded by the first shape, and (c) the incident position of the pulsed laser beam is between the aforementioned films. On the table, it will move in a direction perpendicular to the long axis direction of the beam profile of the pulsed laser beam, and in a manner that partially overlaps the previously irradiated area, the position of the pulsed laser beam and at least the processing object A project that moves by one party, and (d) a project that makes a pulsed laser beam having a light intensity distribution having the aforementioned first shape enter the film at least once, and (e) iteratively performs the aforementioned project (c) and project (d) ) Of the process. 3 5 · A method for producing a polycrystalline film, comprising: (a) a process of preparing a thin processing object made of an amorphous material on a surface, and (b) applying a film on the surface of the film A pulsed laser beam with a long beam profile in one direction is incident on the film, and the film is melted and solidified. The beam enters the region between the edge extending from the long axis direction of the region and the center line, from the edge and From the centerline, crystal grains are generated only in the first strip-shaped region extending in the long axis direction separated by a certain distance, and the light-transmitting film surface is extended in the domain adjacent to the light-recovering surface of the front film surface- 47- (12) 1240957 The first band-shaped region, and the region further outside the first band-shaped region, the crystal grains are smaller than the crystal grains formed in the first band-shaped region, and will be randomly distributed to form a random distribution. Regional engineering. -48--48-
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