TW202330936A - Solution-gated graphene transistor with dual gates - Google Patents
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Abstract
Description
本發明係有關於一種溶液式閘極石墨烯電晶體,尤其係指一種具雙閘極之溶液式閘極石墨烯電晶體。The present invention relates to a solution gate graphene transistor, in particular to a solution gate graphene transistor with double gates.
癌症是全世界已知最具威脅性的疾病之一,最近許多研究表明miRNA-21與癌症密切相關,並且可以在血液中發現它。癌症生物標誌物在癌症診斷中非常重要。眾所周知,預防勝於治療,在疾病的早期發現異常的生物標誌物可以快速且適當的治療。Cancer is one of the most threatening diseases known in the world, and many recent studies have shown that miRNA-21 is closely related to cancer and can be found in blood. Cancer biomarkers are very important in cancer diagnosis. As we all know, prevention is better than cure, and the detection of abnormal biomarkers in the early stage of the disease can lead to rapid and appropriate treatment.
在化學和生物感測器中,由於場效應電晶體的電子感測器具有很高的靈敏度,因此受到青睞。溶液式閘極石墨烯電晶體(solution-gated graphene transistor, SGGT)被認為是很有潛力的感測器,而且SGGT的感測器可以在水溶液中進行量測,這對於生物的感測相當重要。In chemical and biological sensors, electronic sensors with field effect transistors are favored due to their high sensitivity. The solution-gated graphene transistor (SGGT) is considered to be a potential sensor, and the SGGT sensor can be measured in aqueous solution, which is very important for biological sensing .
然而,以做為生物感測器而言,針對不同的目標分析物, SGGT之感測器的靈敏度深深影響著檢測結果。因此,如何提高SGGT之感測器的靈敏度,是業界所需思考的重要課題。However, as a biosensor, for different target analytes, the sensitivity of the SGGT sensor deeply affects the detection results. Therefore, how to improve the sensitivity of the SGGT sensor is an important issue that the industry needs to consider.
有鑑於此,本發明之目的在於提供一種具雙閘極之溶液式閘極石墨烯電晶體,包含:一半導體基板,作為一第一閘極;一介電層,位於所述半導體基板上;一圍阻體,位於所述介電層上,其中所述圍阻體定義一感測區;一對電極組,位於所述介電層之所述感測區上,其中所述電極組作為一通道區,且分別與所述圍阻體外之一源極與一汲極連接;以及一目標溶液,作為一第二閘極,其中所述目標溶液含有目標分析物。In view of this, the object of the present invention is to provide a solution gate graphene transistor with double gates, comprising: a semiconductor substrate as a first gate; a dielectric layer located on the semiconductor substrate; A confining body, located on the dielectric layer, wherein the confining body defines a sensing area; a pair of electrode groups, located on the sensing area of the dielectric layer, wherein the electrode group serves as a channel area, which is respectively connected to a source and a drain outside the enclosure; and a target solution, which serves as a second gate, wherein the target solution contains target analytes.
根據本揭露之一個或多個實施方式,更包含:一複合層結構,位於所述電極組上,具有一石墨烯層以及位於所述石墨烯層上之一石墨烯氧化物層。According to one or more embodiments of the present disclosure, it further includes: a composite layer structure on the electrode assembly, having a graphene layer and a graphene oxide layer on the graphene layer.
根據本揭露之一個或多個實施方式,其中複數個探針分子固定於所述石墨烯氧化物層之表面作為生物受體,且所述複數個探針分子為DNA、RNA、蛋白質、抗體或抗原。According to one or more embodiments of the present disclosure, wherein a plurality of probe molecules are immobilized on the surface of the graphene oxide layer as biological receptors, and the plurality of probe molecules are DNA, RNA, protein, antibody or antigen.
根據本揭露之一個或多個實施方式,其中所述複數個探針分子的密度為10 11~10 13分子/cm 2。 According to one or more embodiments of the present disclosure, the density of the plurality of probe molecules is 10 11 -10 13 molecules/cm 2 .
根據本揭露之一個或多個實施方式,其中所述半導體基板係一n型重摻雜之半導體基板,而所述介電層之材料為Al 2O 3。 According to one or more embodiments of the present disclosure, the semiconductor substrate is a heavily n-doped semiconductor substrate, and the material of the dielectric layer is Al 2 O 3 .
根據本揭露之一個或多個實施方式,其中所述目標分析物為RNA、DNA、蛋白質、抗體或抗原。According to one or more embodiments of the present disclosure, wherein the target analyte is RNA, DNA, protein, antibody or antigen.
根據本揭露之一個或多個實施方式,其中所述RNA為miRNA-21。According to one or more embodiments of the present disclosure, wherein the RNA is miRNA-21.
根據本揭露之一個或多個實施方式,其中所述miRNA-21 的濃度為10 fM~100 pM。According to one or more embodiments of the present disclosure, wherein the concentration of miRNA-21 is 10 fM-100 pM.
根據本揭露之一個或多個實施方式,其中所述電極組為指叉電極,具有複數個彼此對應且平行的條狀部。According to one or more embodiments of the present disclosure, the electrode group is an interdigitated electrode having a plurality of strip-shaped portions corresponding to and parallel to each other.
為便 貴審查委員能對本發明之目的、形狀、構造裝置特徵及其功效,做更進一步之認識與瞭解,茲舉實施例配合圖式,詳細說明如下:In order to facilitate your review committee to further understand and understand the purpose, shape, structure, device features and effects of the present invention, the embodiments are hereby combined with the drawings, and the details are as follows:
首先,要說明的是,在本發明之實施例中,係使用石墨烯氧化物/石墨烯的雙層結構作為SGGT中的通道材料,以檢測miRNA-21等目標分析物。First of all, it should be noted that, in the embodiment of the present invention, the bilayer structure of graphene oxide/graphene is used as the channel material in SGGT to detect target analytes such as miRNA-21.
簡單來說,本發明之實施例利用低壓化學氣相沉積法製備單層石墨烯於銅箔上,經由兩次轉印製備雙層石墨烯(bilayer graphene)於基板上,上層的石墨烯通過低損傷電漿處理(LDPT)被氧化為石墨烯氧化物,以達成原子層氧化(atomic layer oxidation),此層可作為生物接受端。然後,將例如是DNA的單股探針藉由共價鍵進一步固定在石墨烯氧化物的表面,並在固定後與例如是miRNA-21的目標分析物雜合。另外,下層的石墨烯用作電性傳輸層,以傳輸信號。To put it simply, the embodiment of the present invention uses a low-pressure chemical vapor deposition method to prepare single-layer graphene on copper foil, and prepares double-layer graphene (bilayer graphene) on the substrate through two transfers. Lesion plasma treatment (LDPT) is oxidized to graphene oxide to achieve atomic layer oxidation, which serves as a bioreceptor. Then, a single-stranded probe such as DNA is further immobilized on the surface of the graphene oxide through covalent bonding, and hybridizes with a target analyte such as miRNA-21 after immobilization. In addition, the underlying graphene acts as an electrical transport layer to transmit signals.
在本發明之實施例中,經過電流-閘極電壓測量,顯示在目標分析物即miRNA-21之濃度範圍為10 fM~100 pM的情況下,具雙閘極之溶液式閘極石墨烯電晶體的靈敏度為33.65mV/decade。然而,在相同條件下,僅具有一閘極之溶液式閘極石墨烯電晶體的靈敏度只有19.26 mV/decade。也就是說,本發明之實施例所使用的具雙閘極之溶液式閘極石墨烯電晶體,結合了石墨烯氧化物/石墨烯(GO/G)雙層結構作為活性材料,對於miRNA-21等miRNA之檢測具有敏感性和專一性,可進行無標記操作,且有效地將靈敏度提升70﹪。以下,配合圖式詳細說明本發明之實施例。In the embodiment of the present invention, through the current-gate voltage measurement, it is shown that the solution-gate graphene with double gates is electrically conductive when the concentration range of the target analyte, namely miRNA-21, is 10 fM~100 pM. The sensitivity of the crystal is 33.65mV/decade. However, under the same conditions, the sensitivity of the solution-gated graphene transistor with only one gate is only 19.26 mV/decade. That is to say, the solution gate graphene transistor with double gate used in the embodiment of the present invention combines graphene oxide/graphene (GO/G) bilayer structure as active material, for miRNA- The detection of miRNAs such as 21 has sensitivity and specificity, and can be performed without labeling, and the sensitivity can be effectively increased by 70%. Hereinafter, embodiments of the present invention will be described in detail with reference to the drawings.
首先,請一併參考圖1A~1C,圖1A係繪示本發明一實施例之具雙閘極之溶液式閘極石墨烯電晶體的示意圖。圖1B係繪示本發明一實施例之具雙閘極之溶液式閘極石墨烯電晶體中GO/G雙層結構的示意圖。圖1C係繪示本發明一實施例之具雙閘極之溶液式閘極石墨烯電晶體的俯視圖。First, please refer to FIGS. 1A-1C together. FIG. 1A is a schematic diagram of a solution-gate graphene transistor with double gates according to an embodiment of the present invention. 1B is a schematic diagram illustrating a GO/G double-layer structure in a solution gate graphene transistor with double gates according to an embodiment of the present invention. 1C is a top view of a solution gate graphene transistor with double gates according to an embodiment of the present invention.
如圖1A所示,具雙閘極之溶液式閘極石墨烯電晶體100包含一重摻雜之半導體基板10、一金屬氧化物層20、一圍阻體30、指叉電極40a、指叉電極40b、一複合層結構60(以下,亦稱「GO/G雙層結構」)、以及一目標溶液70。在此說明書中,GO/G雙層結構係指石墨烯氧化物層60b/石墨烯層60a的雙層結構。在此要特別說明的是,在本發明之其他實施例中,重摻雜之半導體基板10也可以用其他具導電功能的基板或非重摻雜之半導體基板替代。指叉電極40a、40b也可以用其他非指叉電極的電極替代。金屬氧化物層20也可以用其他介電層替代。As shown in FIG. 1A, a solution
如圖1A所示,在本發明之實施例中,重摻雜之半導體基板10作為一第一閘極,在此說明書中稱為背閘極(back gate)。重摻雜之半導體基板10可以是一n型重摻雜之半導體基板。另外,目標溶液70作為一第二閘極,且含有目標分析物70b。在本發明之實施例中,重摻雜之半導體基板10與目標溶液70即是本說明書中所謂的雙閘極。As shown in FIG. 1A , in an embodiment of the present invention, a heavily doped
如圖1A所示,在本發明之實施例中,金屬氧化物層20位於重摻雜之半導體基板10上。金屬氧化物層20之材料例如是Al
2O
3。
As shown in FIG. 1A , in an embodiment of the present invention, a
如圖1A所示,在本發明之實施例中,圍阻體30位於金屬氧化物層20上,其材料例如是聚二甲基矽氧烷(PDMS)。而且,圍阻體30所圍起來的區域係一感測區,用以容納目標溶液70。As shown in FIG. 1A , in an embodiment of the present invention, the
如圖1A、1C所示,在本發明之實施例中,指叉電極40a、指叉電極40b係位於金屬氧化物層20之感測區上,構成相對應的一對指叉電極組。指叉電極40a與指叉電極40b作為一通道區,且分別與圍阻體30外之一源極50a與一汲極50b連接。在本發明之實施例中,指叉電極40a、指叉電極40b、源極50a與汲極50b乃是由下層5nm的Cr與上層50nm的Au所構成。指叉電極40a、指叉電極40b各具有複數個彼此對應且平行的水平條狀部,寬度為0.3mm,長度為8.8mm。指叉電極40a之水平條狀部與指叉電極40b之垂直條狀部間的距離為0.6mm,同樣地,指叉電極40b之水平條狀部與指叉電極40a之垂直條狀部間的距離為0.6mm,但本發明不以此為限。在本發明之其他實施例中,亦可以根據需求而指叉電極40a、指叉電極40b的尺寸以及相對距離有不同的設計。另外,在本發明之實施例中,圍阻體30之尺寸例如是長10mm與寬10mm,但本發明不以此為限。在本發明之其他實施例中,亦可以根據需求而對圍阻體30之尺寸有不同的設計。As shown in FIGS. 1A and 1C , in an embodiment of the present invention, the interdigitated
如圖1B所示,在本發明之實施例中,複合層結構60係位於指叉電極40a、指叉電極40b上,在此圖中係特別放大複合層結構60並省略其餘部分而進行說明。複合層結構60包含一石墨烯層60a以及位於石墨烯層60a上之一石墨烯氧化物層60b。在本發明之實施例中,石墨烯氧化物層60b係具有一功能化之表面,用以固定複數個探針分子80,例如,複數個探針分子80為經氨基修飾的 DNA 探針,藉由氨基與石墨烯氧化物層60b之-COOH基團反應,而固定於所述功能化之表面並作為生物受體,以捕獲目標溶液70中的目標分析物70b。在本發明之實施例中,複數個探針分子80固定於石墨烯氧化物層60b之功能化表面的密度係介於10
12~10
13分子/cm
2,例如是1.62×10
12分子/cm
2。另外,在本發明之實施例中,石墨烯層60a則作為一信號傳輸層。在本發明之實施例中,目標分析物70b為微小RNA(miRNA),例如是miRNA-21,且miRNA-21 的濃度為10fM~100pM。在此要說明的是,在本發明之實施例中,石墨烯氧化物層60b之表面的功能化可以使用共價和非共價方法進行。
As shown in FIG. 1B, in the embodiment of the present invention, the
請再參考圖1A,要特別說明的是,在本發明之實施例中,目標溶液70係作為一第二閘極,且目標溶液70含有目標分析物70b。當目標溶液70滴入圍阻體30內的感測區時,對目標溶液70與重摻雜之半導體基板10等雙閘極施加電壓,則石墨烯氧化物層60b上的複數個探針分子80會與miRNA-21雜合。Please refer to FIG. 1A again. It should be noted that in the embodiment of the present invention, the
結果,請參考圖2,圖2係表示本發明一實施例之具雙閘極之溶液式閘極石墨烯電晶體與僅具有一閘極之溶液式閘極石墨烯電晶體的靈敏度差異。如圖2所示,曲線1代表的是僅具有一閘極之溶液式閘極石墨烯電晶體,靈敏度為19.26 mV/decade。另外,曲線2代表的是雙閘極之溶液式閘極石墨烯電晶體,靈敏度為33.65 mV/decade。由圖2可知,本發明之實施例的溶液式閘極石墨烯電晶體因為採用了雙閘極,亦即多了一個作為背閘極(back gate)的重摻雜之半導體基板10,使得靈敏度提升了70﹪。As a result, please refer to FIG. 2 . FIG. 2 shows the sensitivity difference between a solution-gate graphene transistor with double gates and a solution-gate graphene transistor with only one gate according to an embodiment of the present invention. As shown in Figure 2, curve 1 represents a solution-gate graphene transistor with only one gate, with a sensitivity of 19.26 mV/decade. In addition, curve 2 represents a solution gate graphene transistor with double gates, with a sensitivity of 33.65 mV/decade. As can be seen from FIG. 2, the solution-type gate graphene transistor of the embodiment of the present invention uses a double gate, that is, one more heavily doped
另外,關於本發明之實施例中具雙閘極之溶液式閘極石墨烯電晶體100的製造方法,說明如下。首先,使用原子層沉積法將 6 nm 的金屬氧化物層20(例如是Al
2O
3膜)沉積到重摻雜之半導體基板10(例如是重 n 摻雜的 Si 基板)上。接著,利用熱蒸鍍法透過遮罩將指叉電極40a、指叉電極40b(例如是5nm之Cr與50nm之Au的複合層)沉積到金屬氧化物層20的預定區域上。然後,使用低壓化學氣相沉積法,另外在一銅箔上生長單層石墨烯。接著,使用聚(甲基丙烯酸甲酯)方法將生長的石墨烯從銅箔轉移到金屬氧化物層20與指叉電極40a、指叉電極40b上。之後,在真空下退火,以去除轉移過程後殘留在金屬氧化物層20與指叉電極40a、指叉電極40b表面的任何有機材料。接下來,通過重複轉移方法將另一個單層石墨烯從銅箔轉移到第一個單層石墨烯上,以獲得堆疊雙層石墨烯(DLG)。之後,對此堆疊雙層石墨烯再次進行退火並進行低損傷電漿處理(LDPT),以獲得複合層結構60,即GO/G雙層結構。
In addition, the method for manufacturing the solution
亦如前所述,在本發明之實施例中,具雙閘極之溶液式閘極石墨烯電晶體100,除了採用雙閘極外,更以石墨烯氧化物層60b/石墨烯層60a的雙層結構作為活性材料,其中,上層經功能化之石墨烯氧化物層60b幾乎完全被氧化,用於與探針分子形成共價鍵,以檢測目標分析物70b,同時下層之石墨烯層60a未被氧化而保留原石墨烯的特性,作為電性傳輸層以傳輸信號,從而形成具雙閘極之溶液式閘極石墨烯電晶體100。也就是說,在本發明之實施例中,透過低損傷電漿處理(LDPT)精確控制石墨烯氧化物層60b/石墨烯層60a的氧化程度,以使石墨烯氧化物層60b與石墨烯層60a具有上述不同的特性。另外,在本發明之其他實施例中,目標分析物70b也可以是其他RNA,或者是DNA、蛋白質、抗體或抗原。在本發明之其他實施例中,探針分子80也可以是其他DNA,或者是RNA、蛋白質、抗體或抗原。Also as mentioned above, in the embodiment of the present invention, the
以上實施方式僅用以說明本發明的技術方案而非限制,儘管參照較佳實施方式對本發明進行了詳細說明,本領域的普通技術人員應當理解,可以對本發明的技術方案進行修改或等同替換,而不脫離本發明技術方案的精神和範圍。The above embodiments are only used to illustrate the technical solutions of the present invention without limitation. Although the present invention has been described in detail with reference to preferred embodiments, those skilled in the art should understand that the technical solutions of the present invention can be modified or equivalently replaced. Without departing from the spirit and scope of the technical solution of the present invention.
10:重摻雜之半導體基板
20:金屬氧化物層
30:圍阻體
40a:指叉電極
40b:指叉電極
50a:源極
50b:汲極
60:複合層結構
60a:石墨烯層
60b:石墨烯氧化物層
70:目標溶液
70b:目標分析物
80:探針分子
100:具雙閘極之溶液式閘極石墨烯電晶體。10: Heavily doped semiconductor substrate
20: metal oxide layer
30:
圖1A係繪示本發明一實施例之具雙閘極之溶液式閘極石墨烯電晶體的示意圖。 圖1B係繪示本發明一實施例之具雙閘極之溶液式閘極石墨烯電晶體中GO/G雙層結構的示意圖。 圖1C係繪示本發明一實施例之具雙閘極之溶液式閘極石墨烯電晶體的俯視圖。 圖2係表示本發明一實施例之具雙閘極之溶液式閘極石墨烯電晶體與僅具有一閘極之溶液式閘極石墨烯電晶體的靈敏度差異。 FIG. 1A is a schematic diagram of a solution gate graphene transistor with double gates according to an embodiment of the present invention. 1B is a schematic diagram illustrating a GO/G double-layer structure in a solution gate graphene transistor with double gates according to an embodiment of the present invention. 1C is a top view of a solution gate graphene transistor with double gates according to an embodiment of the present invention. FIG. 2 shows the sensitivity difference between a solution-gate graphene transistor with double gates and a solution-gate graphene transistor with only one gate according to an embodiment of the present invention.
10:重摻雜之半導體基板 10: Heavily doped semiconductor substrate
20:金屬氧化物層 20: metal oxide layer
30:圍阻體 30: Enclosing body
50a:源極 50a: source
50b:汲極 50b: drain
60:複合層結構 60: Composite layer structure
70:目標溶液 70: target solution
70b:目標分析物 70b: Target analyte
80:探針分子 80: Probe molecule
100:具雙閘極之溶液式閘極石墨烯電晶體 100:Solution gate graphene transistor with double gates
Claims (9)
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