CN108138307A - 电介质薄膜、电容元件及电子部件 - Google Patents
电介质薄膜、电容元件及电子部件 Download PDFInfo
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- CN108138307A CN108138307A CN201680057466.2A CN201680057466A CN108138307A CN 108138307 A CN108138307 A CN 108138307A CN 201680057466 A CN201680057466 A CN 201680057466A CN 108138307 A CN108138307 A CN 108138307A
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- perovskite structure
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- KTUFCUMIWABKDW-UHFFFAOYSA-N oxo(oxolanthaniooxy)lanthanum Chemical compound O=[La]O[La]=O KTUFCUMIWABKDW-UHFFFAOYSA-N 0.000 description 1
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- PBCFLUZVCVVTBY-UHFFFAOYSA-N tantalum pentoxide Inorganic materials O=[Ta](=O)O[Ta](=O)=O PBCFLUZVCVVTBY-UHFFFAOYSA-N 0.000 description 1
- HLLICFJUWSZHRJ-UHFFFAOYSA-N tioxidazole Chemical compound CCCOC1=CC=C2N=C(NC(=O)OC)SC2=C1 HLLICFJUWSZHRJ-UHFFFAOYSA-N 0.000 description 1
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Abstract
本发明提供一种即使将金属氧氮化物中含有的氮量控制为很低,也可以兼备高相对介电常数和高绝缘性的电介质薄膜。该电介质薄膜由具有钙钛矿结构的电介质组合物构成,电介质组合物具有由化学式MazMbOxNy(Ma为选自Sr、Ba、Ca、La、Ce、Pr、Nd、Na中的一种以上的元素,Mb为选自Ta、Nb、Ti、W中的一种以上的元素,O为氧,N为氮)表示的组成,在将Ma占据钙钛矿结构中的A位点时显示的离子价数设为a,将Mb占据钙钛矿结构中的B位点时显示的离子价数设为b时,a和b为6.7≤a+b≤7.3;x、y、z为0.8≤z≤1.2;2.450≤x≤3.493;0.005≤y≤0.700,该电介质组合物为包含Ma及Mb的金属氧氮化物固溶体。
Description
技术领域
本发明涉及一种电介质薄膜、具备电介质薄膜的电容元件以及电子部件。
背景技术
随着近年来电子设备的多功能化,封装在电子电路基板上的电子部件的个数呈现出增大的趋势。在电子设备中,其小型化也在推进,为了兼顾设备的多功能化和小型化,强烈期待提高电子部件的封装密度。为了提高封装密度,需要各种电子部件的高性能化、小型化,作为电子部件之一的薄膜电容器中,对于小型化及高性能化的要求也日益增强。
目前,作为薄膜电容器用途的电介质材料,多使用金属氧化物材料,为了获得具有更高功能的薄膜电子部件,多年以来一直致力于材料特性的改善。但是,通过金属氧化物所实现的电子部件特性的提高正在逐渐达到极限,强烈要求具有更高特性的新材料。
为了进一步提高薄膜电容器的特性,近年来,关于金属氧化物以外的具有高介电特性的材料的开发在不断发展。作为金属氧化物以外的具有高介电特性的材料,可以列举将钙钛矿型晶体结构的氧八面体中的一部分氧原子置换为氮原子的金属氧氮化物材料。另外,钙钛矿结构一般为由ABX3(X:O、N、C、F)所表示的结构体。
专利文献1公开了关于相对介电常数达到11000并超过现有钛酸钡中所获得的相对介电常数的金属氧氮化物的技术。但是,其相对介电常数是由将金属氧氮化物的粉末CIP成形而成的颗粒算出的,不是如普通电介质那样,由金属氧氮化物的颗粒烧结而成的块状烧结体算出的。这样的粉末成形体中难以获得充分的绝缘性。
因此,在专利文献2中,对具有钙钛矿结构的金属氧氮化物的烧结体的相对介电常数进行评价,并说明其频率依赖性较小,但并未就相对介电常数的值进行明确记载。另外,也未对制得的氮氧化物的烧结体是否确保充分的绝缘性进行探讨。
但是,非专利文献1中记载了具有与上述钙钛矿结构不同的钙钛矿型层板结构的酸化物铁电体(ferroelectrics)。在非专利文献1中,具有钙钛矿型层板结构的物质主要分为三组。第一组为被称为Ruddlesden-Popper型且由通式Am+1BmO3m+1表示的物质。作为具体物质,可以例示作为高温超导氧化物的La2-xSrxCuO4等。第二组为被称为Aurevilleus型且由通式Am-1Bi2BmO3m+3表示的物质。作为具体物质,可以列举期待用于铁电体薄膜存储器中的作为Bi系铁电体的SrBi2Ta2O9。第三组为被称为钙钛矿型层板结构且由通式AnBnO3n+2表示的物质。在通式AnBnO3n+2中n=4时,成为由A2B2O7的组成式表示的物质。作为这样的物质,作为代表例可以举出Sr2Ta2O7或La2Ti2O7。
另一方面,存在作为以相同A2B2O7的组成式表示的结构体而具备烧绿石结构的物质。具体而言,可以举出作为磁性体的Dy2Ti2O7。另外,通常已知烧绿石结构虽然与钙钛矿结构的组成式相同,但晶体结构和介电性都相当不同。
另外,非专利文献2中记载了在高温下烧结金属氧氮化物的原料粉末和碳粉末,并得到作为烧结体的金属氧氮化物。
现有技术文献
专利文献
专利文献1:日本特开2013-1625号公报
专利文献2:日本特开昭61-122108号公报
非专利文献
非专利文献1:岛根大学教育学部纪要(自然科学),第36卷,第65~69页,平成14年12月,《具有钙钛矿型相关层状结构的A2B2O7型氧化物铁电体的结晶化学》,秋重幸邦、釜田美纱子;
非专利文献2:Wenbin Dai et al.,Journal of the Ceramic Society ofJapan,115,1,42-46(2007)
发明内容
发明想要解决的技术问题
专利文献2中记载了,获得氧和氮为化学计量比的以组成式ABO2N或ABON2表示且具有钙钛矿结构的金属氧氮化物彼此的固溶体的烧结体,从而实现高的相对介电常数。
认为这是通过向金属氧氮化物的钙钛矿结构的氧离子的位点导入共价结合性强的氮离子,结晶更容易畸变,其结果,显示出高相对介电常数。
但是,通过导入氮离子,从而如果向专利文献2中公开的材料(ABO2N或ABON2)那样,金属氧氮化物中所含的氮的含量增多,则会产生作为电介质组合物起作用所需的绝缘性降低的问题。
因此,在如专利文献2中公开的氮含量较多的材料中,绝缘性容易降低,不能测得准确的相对介电常数的可能性很高。
另一方面,为了提高绝缘性,考虑了降低所导入的氮离子量的对策,但如果导入的氮离子量减少,则难以维持金属氧氮化物的钙钛矿结构,从而生成烧绿石结构或钙钛矿型层状结构等相对介电常数低的金属氧化物相。因此,在导入的氮离子量较少时,会成为金属氧化物和金属氧氮化物的混合体,从而存在难以获得作为具有钙钛矿结构的金属氧氮化物的特征的高相对介电常数,并且难以兼顾高相对介电常数和高绝缘性的问题。
进一步,专利文献2中没有记载可以在少于化学计量比的氮的含量较少的区域中,通过形成具有金属氧化物和金属氧氮化物的中间组成的固溶体,从而兼具高绝缘性和高相对介电常数。
另外,通过气相沉积法等得到的薄膜因其形成方法的差异而具有与如专利文献2中记载的烧结体不同的结构。但是,虽然已知氮含量较多的金属氧氮化物(例如,组成式ABO2N表示的具有钙钛矿结构的物质)的薄膜也显示出高相对介电常数,但是与烧结体相同的理由,在氮含量较少的区域,难以兼顾高相对介电常数和高绝缘性。
因此,本发明是鉴于上述现有的技术问题而完成的,其目的在于提供一种即使将金属氧氮化物中含有的氮量控制为较低,也可以兼顾高相对介电常数和高绝缘性的电介质薄膜、以及具备该电介质薄膜的电容元件。
用于解决技术问题的手段
本发明人等发现,通过制作具有规定组成的电介质薄膜,可以作为固溶体稳定地形成具有钙钛矿结构的金属氧氮化物,从而完成了本发明。
为了解决上述技术问题而完成的本发明的电介质薄膜包含以下方式。
[1]一种电介质薄膜,其特征在于,
该电介质薄膜由包含具有钙钛矿结构的电介质的电介质组合物构成,
上述电介质组合物具有由化学式MazMbOxNy(其中,Ma表示选自Sr、Ba、Ca、La、Ce、Pr、Nd、Na中的一种以上的元素,Mb表示选自Ta、Nb、Ti、W中的一种以上的元素,O表示氧,N表示氮)表示的组成,
在将上述Ma占据上述钙钛矿结构中的A位点时显示的离子价数设为a,将上述Mb占据上述钙钛矿结构中的B位点时显示的离子价数设为b时,上述a和b满足6.7≤a+b≤7.3的关系,
上述化学式的x、y、z为:
0.8≤z≤1.2;
2.450≤x≤3.493;
0.005≤y≤0.700,
该电介质组合物其为包含Ma和Mb的金属氧氮化物固溶体。
[2]一种电介质薄膜,其特征在于,
该电介质薄膜由包含具有钙钛矿结构的电介质的电介质组合物构成,
上述电介质组合物具有由化学式MazMbOxNy(其中,Ma表示选自Sr、Ba、Ca、La、Ce、Pr、Nd、Na中的一种以上的元素,Mb表示选自Ta、Nb、Ti、W中的一种以上的元素,O表示氧,N表示氮)表示的组成,
在将上述Ma占据上述钙钛矿结构中的A位点时显示的离子价数设为a,上述Mb占据上述钙钛矿结构中的B位点时显示的离子价数设为b时,上述a和b满足6.7≤a+b≤7.3的关系,
上述化学式的x、y、z为:
0.8≤z≤1.2;
2.450≤x≤3.493;
0.005≤y≤0.700,
在上述电介质薄膜的X射线衍射图谱中,将表示归属于上述钙钛矿结构的衍射X射线的峰强度中显示出最大强度的峰强度设为100时,不归属于上述钙钛矿结构的衍射X射线的峰强度中显示出最大强度的峰强度为0以上且10以下。
通过制成具有如上所述特征的金属氧氮化物的电介质薄膜,即使将金属氧氮化物中含有的氮量控制为很低,也可以获得高相对介电常数,因此能够兼顾高绝缘性和高相对介电常数。
[3]根据[2]所述的电介质薄膜,其特征在于,归属于上述钙钛矿结构的衍射X射线的峰中显示出最大强度的峰以及不归属于上述钙钛矿结构的衍射X射线的峰中显示出最大强度的峰存在于2θ=30~35°的范围内。
[4]根据[2]或[3]所述的电介质薄膜,其特征在于,不归属于钙钛矿结构的衍射X射线为归属于钙钛矿型层板结构的衍射X射线。
[5]一种电介质薄膜,其特征在于,
在具有由化学式MazMbOxNy(其中,Ma表示位于钙钛矿结构的A位点上的金属离子,Mb表示位于钙钛矿结构的B位点上的金属离子,O表示氧离子,N表示氮离子)表示的钙钛矿结构的电介质薄膜中,
在将上述Ma和Mb各自的平均价数设为a、b时,上述a和b的关系满足a+b=7.0,
上述化学式的x、y、z为:
0.8≤z≤1.2;
2.450≤x≤3.493;
0.005≤y≤0.700,
上述电介质薄膜由Ma和Mb得到的金属氧化物与由Ma和Mb得到的金属氧氮化物的固溶体构成。
通过制成具有如上所述特征的金属氧氮化物的电介质薄膜,从而即使将金属氧氮化物中含有的氮量控制为很低,也可以获得高相对介电常数,因此能够兼顾高绝缘性和高相对介电常数。
[6]优选在上述钙钛矿结构中,将存在于通过CuKα1射线(的波长)进行XRD分析时的2θ=30°~35°的源自由Ma和Mb得到的金属氧氮化物的具有最大强度的峰的强度设为100时,存在于2θ=30°~35°内的源自由Ma和Mb得到的金属氧化物的峰的强度为0以上且10以下。
通过控制在上述范围内,可以增强提高绝缘性的作用。其结果,能够兼顾高的相对介电常数以及更高的绝缘性。
[7]优选地,上述Ma为选自Sr、Ba、Ca、La、Ce、Pr、Nd、Na中的一种以上的元素,Mb为选自Ta、Nb、Ti、W中的一种以上的元素。
通过选定上述元素,可以增强稳定地形成具有钙钛矿结构的金属氧化物和金属氧氮化物的固溶体的作用。其结果,能够兼顾更高相对介电常数和高绝缘性。
另外,作为本发明的优选方案,优选为具有上述电介质薄膜的电容元件。通过使用本发明的电介质组合物,可以获得至今未能得到的具有高静电容量的薄膜电容器等电容元件。
发明效果
根据本发明,可以提供一种即使将金属氧氮化物中含有的氮量控制为较低,也能给兼顾高相对介电常数(例如,1000以上)和高绝缘性(例如,1010Ωcm以上)的电介质薄膜以及电容元件。
附图说明
图1为制造的金属氧氮化物SrTaO2N的X射线衍射图谱(本发明的比较例1)。
图2为制造的金属氧化物Sr2Ta2O7(常温常压)的X射线衍射图谱(本发明的比较例5)。
图3表示制造的金属氧氮化物和金属氧化物的混晶的X射线衍射图谱(本发明的比较例3)。
图4为制造的金属氧化物Sr2Ta2O7(施加应力时)和金属氧氮化物SrTaO2N的固溶体的X射线衍射图谱(本发明的实施例2)。
图5为薄膜电容器的示意图。
符号说明
11…支撑基板
12…下电极
13…电介质膜
14…上电极
具体实施方式
下面,对本发明的实施方式进行说明。本发明的第一观点的电介质薄膜为由具有钙钛矿结构的电介质组合物构成的电介质薄膜。该电介质组合物具有化学式MazMbOxNy(其中,Ma表示选自Sr、Ba、Ca、La、Ce、Pr、Nd、Na中的一种以上的元素,Mb表示选自Ta、Nb、Ti、W中的一种以上的元素,O表示氧,N表示氮)表示的组成。另外,具有钙钛矿结构的电介质为由氧形成的八面体的一部分氧被氮取代而成的氧化物和氮化物的固溶体。
但是,在上述化学式中,在x=2、y=1时,电介质组合物被表示为以化学计量比含有氧和氮的MazMbO2N,其作为钙钛矿结构稳定的金属氧氮化物固溶体而存在。但是,从确保具有钙钛矿结构的金属氧氮化物的绝缘性的观点出发,MazMbO2N中的氮的含量较多。因此,在本实施方式中,在具有这种钙钛矿结构的金属氧氮化物固溶体中,氮的含量(y)小于1。
具体而言,优选上述y为0.005以上,进一步优选为0.300以上,更优选为0.500以上。另一方面,优选y为0.700以下,进一步优选为0.600以下。另外,若y<0.005,则不能充分得到通过为金属氧氮化物固溶体而获得的效果,若y>0.700,则不能得到绝缘性。上述效果为由N的共价结合性引起的晶体畸变获得的高相对介电常数。即使在使“y”为上述范围内的情况下,本实施方式的电介质薄膜也是作为维持了钙钛矿结构的金属氧氮化物固溶体而存在的。
另外,在上述化学式中,为了补偿电荷,对应于氮(价数为-3)的含量(y)减少,在本实施方式中,氧(价数为-2)的含量(x)大于2。
具体而言,优选上述x为2.450以上,进一步优选为2.600以上。另一方面,优选x为3.493以下,进一步优选为3.050以下,更优选为2.750以下。另外,若x<2.450,则不能获得绝缘性,若x>3.493,则不能充分获得通过为金属氧氮化物固溶体而得到的效果。上述效果为由N的共价结合性引起的晶体畸变得到的高相对介电常数。
在上述化学式中,z表示电介质组合物中的Ma和Mb的存在比。在本实施方式中,优选z为0.8以上,进一步优选为0.9以上。另一方面,优选z为1.2以下,进一步优选为1.1以下。另外,若z<0.8,则绝缘性变差,若z>1.2,例如,当Ma为Sr时,会产生SrO等的偏析,存在相对介电常数降低的倾向。
另外,当z>1.0时,优选上述y在0.500以上且0.700以下的范围。
另外,在将Ma占据钙钛矿结构中的A位点时显示的离子价数设为a,将Mb占据钙钛矿结构中的B位点时显示的离子价数设为b时,a及b满足6.7≤a+b≤7.3的关系。
在本实施方式中,上述离子价数a和离子价数b分别表示为平均价数。平均价数采用将A位点或B位点上存在的离子的价数根据其存在比进行平均化而得到的值。例如,针对A位点上以4:1的比存在Sr和La的情况进行说明。钙钛矿结构中的Sr离子的价数为2,钙钛矿结构中的La离子的价数为3。因此,A位点的平均价数a由下述(式1)算出,a为2.2价。
(式1)
(上述情况下的平均价数a)
=2(Sr离子的价数)×4/5(Sr离子的存在比)+3(La离子的价数)×1/5(La离子的存在比)
=8/5+3/5
=11/5
=2.2……(1)
同样地,针对B位点上以4:1的比存在Ta和Ti的情况进行说明。钙钛矿结构中的Ta离子的价数为5,钙钛矿结构中的Ti离子的价数为4。因此,B位点的平均价数b由下述(式2)算出,b为4.8价。
(式2)
(上述情况下的平均价数b)
=5(Ta离子的价数)×4/5(Ta离子的存在比)+4(Ti离子的价数)×1/5(Ti离子的存在比)
=20/5+4/5
=24/5=4.8……(2)
另外,在本申请的平均价数的合计的计算中,即使在富含A位点或富含B位点时,即,在z≠1时,也作为z=1处理。例如,在上述情况下,即使在z=1.2时,平均价数的合计(a+b)也为2.2+4.8=7.0。
在本实施方式中,通过使作为平均价数表示的离子价数a和离子价数b之和“a+b”在6.7~7.3的范围内,从而MaMbO2N在常温常压下形成的钙钛矿结构稳定化,因此,氮含量小于MaMbO2N的MazMbOxNy也变得容易形成钙钛矿结构。例如,当a+b=6.0时,上述MaMbO2N的钙钛矿结构未稳定化,因此不能得到均匀的固溶体。另一方面,当a+b=8.0时,MaMbON2的钙钛矿结构被稳定化。与MaMbO2N的钙钛矿结构相比,MaMbON2的钙钛矿结构需要更多的N,因此,更难获得绝缘性。
Ma元素为选自Sr、Ba、Ca、La、Ce、Pr、Nd、Na中的一种以上的元素。另外,Mb元素为选自Ta、Nb、Ti、W中的一种以上的元素。特别优选Ma为Sr,Mb为Ta。
通过采用如上所述的组合,容易获得具有钙钛矿结构的金属氧氮化物的固溶体。
本发明的第二观点的电介质薄膜为由包含具有钙钛矿结构的电介质的电介质组合物构成的电介质薄膜。该电介质组合物具有化学式MazMbOxNy(其中,Ma表示选自Sr、Ba、Ca、La、Ce、Pr、Nd、Na中的一种以上的元素,Mb表示选自Ta、Nb、Ti、W中的一种以上的元素,O表示氧,N表示氮)表示的组成,关于化学式中的“x”、“y”和“z”,与第一观点的电介质薄膜中的说明重复,故省略。进一步,关于离子价数a、离子价数b以及它们的和(a+b),也与第一观点的电介质薄膜中的说明重复,故省略。
第二观点的电介质薄膜中,在其X射线衍射图谱中,出现归属于钙钛矿结构的衍射X射线的峰。这是归属于该电介质薄膜中包含的电介质的峰,在本实施方式中,其为归属于具有钙钛矿结构的金属氧氮化物的峰。因此,电介质薄膜通过具备具有钙钛矿结构的规定组成的金属氧氮化物,从而包含该金属氧氮化物的电介质薄膜可以兼顾高相对介电常数和高绝缘性。另外,在电介质薄膜的X射线衍射图谱中,可以在能够兼顾高相对介电常数和高绝缘性的范围内,存在不归属于钙钛矿结构的衍射X射线的峰。
具体而言,将归属于钙钛矿结构的衍射X射线的峰强度中显示出最大强度的峰强度设为100时,不归属于钙钛矿结构的衍射X射线的峰强度中显示出最大强度的峰强度为0以上且10以下。当该峰强度大于0时,在这样的电介质薄膜中,具有钙钛矿结构的相和不具有钙钛矿结构的相共存,成为所谓的混晶。但是,与具有钙钛矿结构的物质的存在比例相比,不具有钙钛矿结构的物质的存在比例非常小,因此,能够兼顾高相对介电常数和高绝缘性。
作为钙钛矿结构以外的结构,没有特别限制,但在混晶状态具有钙钛矿结构的物质优选为能够维持该钙钛矿结构的物质。在本实施方式中,钙钛矿结构以外的结构优选为钙钛矿型层板结构。作为用于形成电介质薄膜的原料(例如,成膜用靶材),优选具有钙钛矿型层板结构的物质,此外,在上述化学式表示的组成范围内,钙钛矿结构和钙钛矿型层板结构可以在薄膜中作为混晶而共存,这一点后面将予以叙述。具有钙钛矿型层板结构的化合物虽然未显示出高相对介电常数,但若钙钛矿型层板结构的峰强度在上述范围内,则能够兼顾高相对介电常数和高绝缘性。
另外,如上所述,烧绿石结构由与钙钛矿型层板结构相同的组成式表示,但在存在具有烧绿石结构的物质时,存在具有钙钛矿结构的物质难以维持该钙钛矿结构,并且具有烧绿石结构的物质和具有钙钛矿结构的物质不能共存的倾向。因此,当电介质薄膜包含具有烧绿石结构的物质时,不能获得高相对介电常数和高绝缘性。
例如,当未导入氮的金属氧化物Ma2Mb2O7具有钙钛矿型层板结构时,通过将这样的金属氧化物作为原料,从而包含Ma及Mb的金属氧氮化物的固溶体容易维持钙钛矿结构。具体而言,Sr2Ta2O7、Sr2Nb2O7、Ca2Nb2O7、Na2W2O7、La2Ti2O7、Ce2Ti2O7、Pr2Ti2O7、Nd2Ti2O7具有钙钛矿型层板结构。虽然不存在Ba2Ta2O7,但(SrBa)2Ta2O7具有钙钛矿型层板结构。
另一方面,作为除作为上述Ma及Mb所示例的元素以外的元素的组合的Pb2Ta2O7、Cd2Ta2O7、Y2Si2O7、Cr2Ti2O7、Tb2Ge2O7、Sc2Si2O7等具有烧绿石结构。因此,即使想要使用这些金属氧化物形成金属氧氮化物的固溶体,也不会成为钙钛矿结构。
另外,优选归属于钙钛矿结构的衍射X射线的峰强度中显示出最大强度的峰、以及不归属于钙钛矿结构的衍射X射线的峰强度中显示出最大强度的峰均存在于2θ为30~35°的范围内。
本发明的第三观点的电介质薄膜为具有由化学式MazMbOxNy(其中,Ma表示位于钙钛矿结构的A位点上的金属离子,Mb表示位于钙钛矿结构的B位点上的金属离子,O表示氧离子,N表示氮离子)表示的钙钛矿结构的电介质薄膜。与第一及第二观点的电介质薄膜相同,上述化学式的x、y、z为0.8≤z≤1.2,2.450≤x≤3.493,0.005≤y≤0.700。“x”、“y”及“z”的优选范围也与第一及第二观点的电介质薄膜相同。
另外,在将Ma和Mb各自的平均价数设为a和b时,上述a和b的关系满足a+b=7.0。另外,平均价数a及平均价数b可以与第一及第二观点的电介质薄膜同样地求取。通过使上述a+b=7.0,MaMbO2N在常温常压下形成的钙钛矿结构稳定化,因此,氮含量少于MaMbO2N的MazMbOxNy也容易形成钙钛矿结构。当a+b=6.0时,上述MaMbO2N的钙钛矿结构未稳定化,因此不能获得均匀的固溶体。另一方面,当a+b=8.0时,MaMbON2的钙钛矿结构稳定化。与MaMbO2N的钙钛矿结构相比,MaMbON2的钙钛矿结构需要更多N,因此更难以获得绝缘性。
而且,第三观点的电介质薄膜的特征在于,其由Ma和Mb得到的金属氧化物与由Ma和Mb得到的金属氧氮化物的固溶体构成。在此,“由Ma和Mb得到的金属氧化物与由Ma和Mb得到的金属氧氮化物的固溶体”表示具有由Ma和Mb得到的金属氧化物与由Ma和Mb得到的金属氧氮化物以规定的比例混合而成的组成的固溶体。
换而言之,“由Ma和Mb得到的金属氧化物与由Ma和Mb得到的金属氧氮化物的固溶体”表示由Ma和Mb得到的金属氧化物与由Ma和Mb得到的金属氧氮化物的中间组成。
例如,当由Ma和Mb得到的金属氧化物用Ma2Mb2O7表示,由Ma和Mb得到的金属氧氮化物用MaMbO2N表示时,“由Ma和Mb得到的金属氧化物与由Ma和Mb得到的金属氧氮化物的固溶体”的组成由MazMbOxNy表示,表示“O”的含量的“x”在2.450~3.493的范围内。另外,表示“N”的含量的“y”在0.005~0.700的范围内。
与此相对,当金属氧化物和金属氧氮化物不是固溶体而仅为混合状态时,低介电常数的上述金属氧化物的相对介电常数影响增强,因此,作为电介质组合物难以获得高相对介电常数。
因此,通过制成具有规定组成的“由Ma和Mb得到的金属氧化物与由Ma和Mb得到的金属氧氮化物的固溶体”,可以生成如上所述的相对介电常数低且具有烧绿石结构或钙钛矿型层状结构的金属氧化物相,并抑制电介质组合物成为金属氧氮化物和金属氧化物的混合体,能够兼顾高相对介电常数和高绝缘性。
另外,在上述金属氧化物和金属氧氮化物的固溶体所具有的钙钛矿结构中,将通过CuKα1射线(的波长)进行XRD分析时的存在于2θ=30°~35°的源自金属氧氮化物MaMbO2N的具有最大强度的峰的强度设为100时,如图4所示,存在于2θ=30°~35°内的源自金属氧化物的峰的强度优选接近0,更优选为0以上且10以下。在此,源自金属氧化物的峰是指形成薄膜时使用的原料的结构引起的峰。
通过制成这样的电介质薄膜,可以获得更高的相对介电常数和绝缘性。另外,如图3所示,当源自金属氧化物的强度大于10时,提高绝缘性的效果较小。另外,图1~4中记载的黑圈●为源自金属氧氮化物的峰(钙钛矿结构),白圈○为源自金属氧化物的峰(钙钛矿型层板结构)。
本实施方式的电介质薄膜为使用薄膜形成法等,对构成电介质薄膜的元素进行沉积而形成的电介质沉积膜。当作为这样的电介质沉积膜而形成时,与烧成粉体而得到的烧结体不同,形成于基板上时,会受到应力的影响,或者不易产生氧缺陷,因此,即使是在氮含量少于具有钙钛矿结构的金属氧氮化物的组成的区域,仍可以兼顾高绝缘性和高相对介电常数。
另外,电介质薄膜的厚度优选为10nm~2μm。若低于10nm,则容易产生绝缘击穿(dielectric breakdown),若超过2μm,则相对于更廉价的BaTiO3等金属氧化物电介质薄膜的产业优势减弱。
下面,对本实施方式的电容元件进行说明。此处所说的电容元件是指利用介电性的元件,包括电容器、热敏电阻器、滤波器、双工器、谐振器、振荡器、天线、压电元件、晶体管(栅极使用电介质绝缘膜)、铁电体存储器等。
另外,本发明的电介质薄膜可以在不损害本发明的效果的范围内含有其它元素。另外,也可以含有制造工序及保管条件下不可避免地导入的其它元素。
下面,作为电容元件,对包含上述电介质薄膜且包含在上述电容器中的薄膜电容器进行具体说明。作为薄膜电容器,对其结构没有明确的定义,但一般用于与层叠型电容器相比其电介质层数较少或为一层,且需要进一步的小型化及低背化的情况。因层数受限,因此多数情况下薄膜电容器要求具有更高的相对介电常数,可以说为本发明特别优选的器件。
图5中示出作为本实施方式的电容元件的一个例子的薄膜电容器的示意图。图5所示的薄膜电容器在支撑基板11上依次形成下电极12、电介质膜13,在电介质膜13的表面上具备作为薄膜电容器的另一电极而起作用的上电极14。用于形成上电极14的材料只要具有导电性即可,没有特别限定,可以利用与下电极12相同的材料形成上电极14。
在此,各层的厚度、形状等可以根据用途调整,另外,各层无需限定为一层。例如,上电极14的膜厚可以作为电极起作用,优选为0.01μm以上。当膜厚为0.01μm以下时,导电性恶化,因而作为上电极14不优选。
下面,针对本实施方式的电介质薄膜的制造方法进行说明。
首先,对将金属氧氮化物作为薄膜而成膜的方法进行说明。作为可以用于使用了本发明的组成的金属氧氮化物的成膜的成膜方法,只要可以获得满足上述化学式的膜的方法即可,没有特别限制,可以例示各种薄膜形成法,例如,真空蒸镀法、溅射法、PLD(脉冲激光沉积法)、MO-CVD(有机金属化学气相沉积法)、MOD(有机金属分解法)或溶胶-凝胶法、CSD(化学溶液沉积法)等。在薄膜形成法中,优选溅射法、化学气相沉积法、PLD等公知的气相沉积法。
另外,有时形成电介质薄膜时所使用的原料(蒸镀材料、各种靶材材料、有机金属材料等)中包含微少的杂质或副成分,但只要不是大幅降低绝缘性的杂质,都不是特别的问题。
在本实施方式中,针对作为成膜方法之一的PLD法进行说明。作为可以用于电介质膜13的成膜的成膜法的一个例子的PLD法,是将包含目标膜的构成元素的靶材设置在成膜室内,在该靶材表面上照射脉冲激光,并通过其强大的能量使靶材表面瞬间蒸发,从而生成羽烟,并在与靶材相对而配置的基板上沉积蒸发物以制成薄膜的方法。
作为靶材,除包含膜构成元素的金属氧化物烧结体之外,只要为包含膜构成元素的物质,也可以使用合金、氮化物烧结体、金属氧氮化物烧结体等。另外,优选在靶材中各元素以所使用的脉冲激光径的尺度平均分布,不过在对获得的金属氧氮化物膜的质量没有影响的范围内,无需特别均匀。靶材也不一定为一个,也可以准备多个包含一部分膜构成元素的靶材用于成膜。靶材的形状可以根据所使用的成膜装置适当选择最佳的形状即可。
在本实施方式中,作为靶材,可以使用通过一般的固相法所制造的包含膜构成元素的金属氧化物烧结体等。
进一步,在本实施方式中,为了获得金属氧氮化物膜,需要进行膜的氧氮化。作为氮氧化方法,可以使用在金属氧化物膜的成膜中将氮自由基导入成膜室中的方法;利用使用氮气等的反应性溅射的方法;使用通过等离子氮化而被活化了的氮的等离子处理等。根据这样的方法,无需使用具有毒性的气体就可以向金属氧化物薄膜的晶体结构内导入氮。或者,可以不经由金属氧化物薄膜,而直接在基板上构成金属氧氮化物。另外,也可以使用氮化膜的部分氧化处理等。在本实施方式中,使用金属氧化物的原料成膜时,优选导入用于氮化的氮,以获得金属氧氮化物。
下面,作为实施方式更为详细的一个例子,对具有SrTaO3.2N0.2组成的电介质薄膜的成膜方法进行说明。作为靶材,可以使用Sr2Ta2O7的烧结体靶材。在本实施方式中,作为基板,优选使用容易获得且便宜的Si单晶基板。在Si单晶基板上依次成膜SiO2、TiOx、Pt,形成Pt下电极。接着,例如,在该Pt下电极上,利用PLD法以200nm的厚度形成电介质膜即可。另外,为了露出下电极的一部分,使用金属掩膜,在下电极上形成部分未成膜电介质膜的区域。
在本实施方式中,为了使膜结晶化,优选成膜时利用红外激光加热基板至600℃~800℃从而进行成膜。此时,若基板温度过低,则不能结晶,若温度过高,则冷却时因基板和膜的热膨胀差而会产生开裂等,因此需要注意。但是,成膜时基板温度的最佳值会根据构成要素、组成而不同,因此,根据这些来选择最佳条件即可,温度范围不限于上述范围。
已知金属氧氮化物的居里温度很高,而成膜温度一般为居里温度以下,因此,成膜后从成膜温度降温至室温时不会产生结构相变。因此,与居里温度为100℃左右的钛酸钡薄膜相比,金属氧氮化物的薄膜具有难以产生裂纹的特征。
另外,成膜时可以使用各种气体种类及气压。由此得到的膜的状态也依赖于成膜室的大小或气体导入管的位置。即,不是使用相同分压就能够获得相同的膜。因此,需要注意的是,作为Sr离子(即Ma)和Ta离子(即Mb)的比,该比会根据气压而变化,因此,可以根据装置以获得所期望的组成比的方式调整气压。特别是金属氧氮化物中,由于其组成中包含O和N,因此还需要注意氧分压和氮分压之比。我们也可以能够获得所期望的组成的方式,根据装置调节分压比及全压。
在如SrTaO3.2N0.2那样含量氮较少的区域,也可以在使用上述靶材成膜形成的金属氧化物薄膜之后,导入氮自由基并对金属氧化物膜进行氮化处理。成膜试样中的氮量可以通过X射线光电子光谱法来确认。关于氮的定量,也可以使用X射线光电子分光装置的内部标准,但优选从AlN等氮化物单晶晶片算出灵敏度因数来校正定量值。氧化或氮化进度因构成要素而不同,因此氮自由基导入量可以根据所选择的元素组适当调整。
这样,在本实施方式中,可以将如上述方式成膜的SrTaO3.2N0.2氮氧化物膜用作电介质膜层,并通过溅射法在其上面形成Pt以作为上电极并得到薄膜电容器。
对于上述薄膜电容器的静电容量,可以在上电极以及下电极上通过探针连接导线,并使用阻抗分析仪测定。测定上述静电容量之后,使用扫描型电子显微镜观察金属氧氮化物膜截面,从该观察图像测定金属氧氮化物膜的厚度d。使用下述关系式(3),由如上得到的静电容量C、金属氧氮化物膜的厚度d、上电极及下电极的重叠面積S计算金属氧氮化物膜的相对介电常数(ε)。
(式3)
C=ε0ε(S/d)……(3)
在此,ε0为真空的介电常数。为了在薄膜电容器中获得高静电容量,优选相对介电常数更高。
另外,本发明不受上述实施方式及后述实施例限定。另外,实施方式及实施例中的构成要素中包含本领域技术人员容易想到的物质、实质相同的物质、所谓同等范围内的物质。进一步,实施方式及实施例中公开的构成要素可以适当组合,也可以适当选择使用。
近年来,为了应对高频及小型化,电容元件的形式多种多样,不能对其全部进行描述。本发明的电容元件是指积极利用其介电特性的元件、或者其介电特性在为了发挥功能的构成上必需的元件,不包含偶然具有容量成分的其它电子器件。
下面,示出本发明的实施例、比较例。
[实施例1~实施例7、比较例1~比较例5]
实施例1~实施例7及比较例4进行了薄膜化。作为用作成膜用靶材的烧结体的原料,使用了SrCO3、Ta2O5、La2O3、TiO2、Na2CO3、WO3。以成为Sr2Ta2O7、La2Ti2O7、Na2W2O7的方式分别秤量,并在使用了乙醇为溶剂的湿式球磨机中混合16小时。用恒温干燥机,在80℃下对得到的混合浆料干燥12小时。利用研钵轻轻粉碎得到的混合物,放入陶瓷制的坩埚,利用电炉,在1000℃、大气气氛中热处理2小时,得到煅烧物。
再利用使用了乙醇用作溶剂的湿式球磨机将得到的煅烧物粉碎16小时,用恒温干燥机,在80℃下干燥粉碎后的浆料12小时,得到粉碎物。向得到的粉碎物中添加以溶液中固形物换算为0.6重量%的聚乙烯醇溶液作为粘合剂并混合,得到了造粒物。将造粒物成型为直径约23mm、高约9mm的圆柱形状,得到了成型物。利用电炉,在大气气氛中1400℃下,烧成成型物2小时,对该烧结物的上面及下面进行镜面研磨使其高度为5mm,得到成膜用靶材。此时,得到的靶材均具有钙钛矿型层板结构,其相对密度为96~98%。
将上述那样得到的成膜用靶材设置在成膜装置中,与靶材相对的方式,设置在表面具有Pt膜作为下电极的Si基板。实施例1~实施例7利用导入氮自由基的PLD法成膜至厚度为200nm。此时,通过控制氧及氮的气体压力,可以获得表1所示的期待结构。由得到的样品的X射线衍射图谱确认了薄膜已结晶。另一方面,比较例4以直接反应氧化物靶材的晶体结构的方式在接近真空条件进行成膜,然后掺杂了N(氮)。
比较例1~比较例3及比较例5与合成上述靶材的顺序相同地,首先合成了金属氧化物Sr2Ta2O7、La2Ti2O7、Na2W2O7。然后,通过如非专利文献2中记载的碳热还原法进行了氮化。利用一般的氨气氛也可以进行氮化,不管通过碳热还原法,可以通过相当的C添加量来控制导入的N量。
使混炼了碳的金属氧化物粉末颗粒化并进行了热处理。热处理是利用可以减压的分批式炉,充分降低一次炉内压力之后,利用大气压的N2气氛充满炉内,在1400℃进行,从而得到烧结体。氮化后未发现C残留。使用溅射器在得到的样品上形成Pt电极,并评价电性能。另外,在比较例5中,不混炼碳,而直接将金属氧化物粉末颗粒化从而进行了上述热处理。
使用LECO公司制造的TC600,通过脉冲加热熔融提取法(红外吸收法)对实施例1~实施例7及比较例1~比较例5的样本的N及O量进行定量。另外,由XPS的化学位移判定金属离子的价数,与原料相比,价数未产生变化。
关于实施例1~实施例7及比较例1~比较例5,将其晶体结构和绝缘性及相对介电常数(ε)总结于表1。
相对介电常数(ε)记作在电压1Vrms/μm、频率1kHz下所评价的值。另外,用于评价相对介电常数的上电极通过以直径100μm的尺寸蒸镀Ag而形成。另外,作为相对介电常数(ε),表1中仅记载了tanδ低于100%的样品的数值,tanδ为100%以上的样品则认为无法评价介电性,将相对介电常数(ε)视为×(未观察到,not observed)。
另外,通过CuKα1射线(的波长)测定XRD图谱。
通过测定电阻值来评价绝缘性。测定电阻值时,使用ADVANTESTR8340A并施加1V/μm电压以进行测定。表1中,将电阻值为1010Ωcm以上的样品的绝缘性记为○(良好,good),将小于该值的记为×(不好,bad)。
【表1】
“*”仅限于金属氧化物具有钙钛矿型层板结构的情况下,表示将金属氧氮化物的主峰强度设为100时的金属氧化物的主峰的强度比。
在表1中的记载有“钙钛矿固溶体”的列中,对上述金属氧化物强度比为0以上且10以下的样品记为○(满足,satisfied)。另一方面,金属氧化物强度比大于10的样品中,源自金属氧氮化物的钙钛矿结构未出现在图谱上,判断其未成为与氧化物的固溶体,从而记作×(不满足,not satisfied)。
比较例1为金属氧氮化物SrTaO2.000N1.000的烧结体,由组成分析和XRD分析也说明了这一点。图1所示的具有明确的X射线峰的比较例1虽然具有钙钛矿结构,但N量较多,因此,可以确定不能确保绝缘性。另外,比较例2为烧结体,并可以确定即使在将金属氧氮化物的主峰强度设为100时的金属氧化物的主峰强度比为12的情况下,也不能确保绝缘性。
比较例5为具有钙钛矿型层板结构的金属氧化物Sr2Ta2O7的烧结体,由组成分析和XRD分析也说明了这一点。得到的明确的XRD图谱示于图2。比较例5虽然可以得到充分的绝缘性,但ε的值很低,仅为50。
另外,比较例3为具有金属氧氮化物SrTaO2.000N1.000和金属氧化物Sr2Ta2O7的中间组成的烧结体。比较例3未成为固溶体,因此,也不能得到充分的绝缘性。其XRD图谱示于图3。由图3,存在源自金属氧氮化物的钙钛矿结构的峰和源自金属氧化物的钙钛矿型层板结构的峰,可知为这些相的混晶状态。图3中所示的黑圈●为源自金属氧氮化物的峰,白圈○为源自金属氧化物的峰。强度比是使用这2点的峰算出。
比较例4为在将具有钙钛矿型层板结构的Sr2Ta2O7成膜后掺杂N而成的薄膜。在比较例4中,几乎未形成具有钙钛矿结构的金属氧氮化物的固溶体,钙钛矿型层板结构的存在比例保持很高。其结果,在与实施例相同的形状下评价电性能,但没有获得绝缘性。
与此相对,在实施例1中,充分形成具有钙钛矿结构的金属氧氮化物固溶体,得到了充分的绝缘性。相对介电常数ε的值也较高,达2100。
同样地,在实施例2~7中,也形成具有钙钛矿结构的金属氧氮化物固溶体,并得到充分的绝缘性和高介电性。特别是实施例2显示出高达2200的相对介电常数ε。将实施例2的XRD图谱示于图4。可以确定,虽然为与图3所示的比较例3相同的组成比,但可以获得钙钛矿结构。
另外,可以确定,如果是如实施例5那样的将强度比控制为10的具有钙钛矿结构的相和具有钙钛矿型层板结构的相的混晶状态的薄膜,则能够确保高绝缘性和高相对介电常数ε。由此可知,通过将金属氧氮化物的主峰强度设为100时的金属氧化物的主峰强度比为10以下,从而可以兼顾高相对介电常数和高绝缘性。
[实施例8~实施例15、比较例6~比较例7]
实施例8~15中也使用与实施例1相同的方法,制成金属氧化物的靶材之后进行薄膜化(薄膜时进行氮化)从而来进行合成。另外,各靶材以薄膜的组成如表2所示的方式进行调整。另外,表2中的Ma及Mb栏中记入两种元素的样品中,为从左起依次为80%、20%的混合比。例如,在实施例8的情况下,以A位点上的Sr为80%、Ba为20%的方式,调整原料SrCO3和BaCO3的比,从而制造了靶材(Sr0.8Ba0.2)2Ta2O7。此时,Sr离子和Ba离子均为2价,因此a=2。另外,在实施例15的情况下,也与实施例8相同地制造。在实施例15的情况下,以A位点上的La为80%、Na为20%;B位点上的Ti为80%,W为20%的方式,调整原料SrCO3、Na2CO3、TiO2、WO3的比,从而制造靶材(La0.8Na0.2)2(Ti0.8W0.2)2O7。此时,La离子为3价,Na离子为1价,Ti离子为4价,W离子为6价,因此,a及b如下。
a=3×0.8+1×0.2=2.4+0.2=2.6
b=4×0.8+6×0.2=3.2+1.2=4.4
使用制成的靶材制造了薄膜。对得到的样品进行电性能评价。结果总结于表2。ε记载了在电压1Vrms/μm、频率1kHz下评价的值。实施例8~实施例15的ε均显示高达1000以上的值。
另一方面,比较例6及比较例7使用本发明以外的组成进行合成,从而制造了成膜用靶材。得到的金属氧化物的靶材均为烧绿石结构。尝试了以成为具有钙钛矿结构的金属氧氮化物固溶体的方式进行成膜,但得到的薄膜不具有钙钛矿结构,且没有获得绝缘性。
【表2】
“*”仅限于金属氧化物具有钙钛矿型层板结构的情况,表示将金属氧氮化物的主峰强度设为100时的金属氧化物的主峰的强度比。
[实施例16~实施例19、比较例8~比较例9]
实施例16~实施例19、比较例8~比较例9也使用与实施例1相同的方法,制造了金属氧化物的靶材之后,进行薄膜化(薄膜时进行氮化)来合成。各靶材以薄膜组成为表3所示的组成的方式进行调整。对得到的样品进行电性能评价。结果总结于表3。ε记载了在电压1Vrms/μm、频率1kHz下评价的值。
【表3】
“*”仅限于金属氧化物具有钙钛矿型层板结构的情况,表示将金属氧氮化物的主峰强度设为100时的金属氧化物的主峰的强度比。
由表3可知,比较例8不能获得绝缘性。另一方面,比较例9虽然可以得到绝缘性,但介电常数值较低。观察比较例9的微细结构,结果发现了SrO的偏析。
[实施例20~21及比较例10~比较例11]
实施例20~实施例21、比较例10~比较例11也使用与施例1相同的方法,在制造了金属氧化物的靶材之后,进行薄膜化(薄膜时进行氮化)来进行合成。各靶材以薄膜组成为表4所示的组成的方式进行调整。对得到的样品进行了电气性能评价。结果总结于表4。
【表4】
“*”仅限于金属氧化物具有钙钛矿型层板结构的情况,表示将金属氧氮化物的主峰强度设为100时的金属氧化物的主峰的强度比。
由表4可以确定,比较例10及11中不能获得绝缘性,也无法评价介电性。
产业上的可利用性
根据本发明,电介质薄膜在N小于化学计量比的区域中也具有与N为化学计量比的晶体结构相同的晶体结构,因此,可以提供显示高电阻及高介电常数的电介质元件。特别是可以为要求小型、应对高温及高频选择性的产品提供优质的电介质薄膜及电容元件。
Claims (10)
1.一种电介质薄膜,其特征在于,
该电介质薄膜由具有钙钛矿结构的电介质组合物构成,
所述电介质组合物具有由化学式MazMbOxNy表示的组成,
其中,Ma表示选自Sr、Ba、Ca、La、Ce、Pr、Nd、Na中的一种以上的元素,Mb表示选自Ta、Nb、Ti、W中的一种以上的元素,O表示氧,N表示氮,
在将所述Ma占据所述钙钛矿结构中的A位点时所显示的离子价数设为a,将所述Mb占据所述钙钛矿结构中的B位点时所显示的离子价数设为b时,所述a和b满足6.7≤a+b≤7.3的关系,
所述化学式的x、y、z为:
0.8≤z≤1.2
2.450≤x≤3.493
0.005≤y≤0.700
所述电介质组合物为包含Ma及Mb的金属氧氮化物固溶体。
2.一种电介质薄膜,其特征在于,
该电介质薄膜由包含具有钙钛矿结构的电介质的电介质组合物构成,
所述电介质组合物具有由化学式MazMbOxNy表示的组成,
其中,Ma表示选自Sr、Ba、Ca、La、Ce、Pr、Nd、Na中的一种以上的元素,Mb表示选自Ta、Nb、Ti、W中的一种以上的元素,O表示氧,N表示氮,
在将所述Ma占据所述钙钛矿结构中的A位点时显示的离子价数设为a,将所述Mb占据所述钙钛矿结构中的B位点时显示的离子价数设为b时,所述a及b满足6.7≤a+b≤7.3的关系,
所述化学式的x、y、z为:
0.8≤z≤1.2;
2.450≤x≤3.493;
0.005≤y≤0.700,
在所述电介质薄膜的X射线衍射图谱中,将归属于所述钙钛矿结构的衍射X射线的峰强度中显示最大强度的峰强度设为100时,不归属于所述钙钛矿结构的衍射X射线的峰强度中显示最大强度的峰强度为0以上且10以下。
3.根据权利要求2所述的电介质薄膜,其特征在于,
归属于所述钙钛矿结构的衍射X射线的峰中显示最大强度的峰以及不归属于所述钙钛矿结构的衍射X射线的峰中显示最大强度的峰存在于2θ=30°~35°的范围内。
4.根据权利要求2或3所述的电介质薄膜,其特征在于,
不归属于所述钙钛矿结构的衍射X射线为归属于钙钛矿型层板结构的衍射X射线。
5.一种电介质薄膜,其特征在于,
在具有由化学式MazMbOxNy表示的钙钛矿结构的电介质薄膜中,其中,Ma表示位于钙钛矿结构的A位点上的金属离子,Mb表示位于钙钛矿结构的B位点上的金属离子,O表示氧离子,N表示氮离子,
在将所述Ma和Mb各自的平均价数设为a、b时,所述a和b的关系满足a+b=7.0,并且
所述化学式的x、y、z为:
0.8≤z≤1.2;
2.450≤x≤3.493;
0.005≤y≤0.700,
所述电介质薄膜由Ma和Mb得到的金属氧化物与由Ma和Mb得到的金属氧氮化物的固溶体构成。
6.根据权利要求5所述的电介质薄膜,其特征在于,
在所述钙钛矿结构中,将存在于通过CuKα1射线进行XRD分析时的2θ=30°~35°的源自由Ma和Mb得到的金属氧氮化物的具有最大强度的峰的强度设为100时,存在于2θ=30°~35°内的源自由Ma和Mb得到的金属氧化物的峰的强度为0以上且10以下,其中,CuKα1射线具有的波长。
7.根据权利要求5或6所述的电介质薄膜,其特征在于,
所述Ma为选自Sr、Ba、Ca、La、Ce、Pr、Nd、Na中的一种以上的元素,Mb为选自Ta、Nb、Ti、W中的一种以上的元素。
8.一种电容元件,其中,
具有权利要求1~7中任一项所述的电介质薄膜。
9.一种电子部件,其中,
具有权利要求1~7中任一项所述的电介质薄膜。
10.一种电子部件,其中,
具有权利要求8所述的电容元件。
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CN114423722A (zh) * | 2019-09-12 | 2022-04-29 | 国立大学法人北海道大学 | 烧结体和其制造方法以及电介质组合物 |
CN114423722B (zh) * | 2019-09-12 | 2023-11-24 | 国立大学法人北海道大学 | 烧结体和其制造方法以及电介质组合物 |
CN114823135A (zh) * | 2021-01-20 | 2022-07-29 | Tdk株式会社 | 电介质组合物及电子部件 |
CN114853472A (zh) * | 2021-01-20 | 2022-08-05 | Tdk株式会社 | 电介质组合物及电子部件 |
US11873255B2 (en) | 2021-01-20 | 2024-01-16 | Tdk Corporation | Dielectric composition and electronic component |
CN114914085A (zh) * | 2021-02-09 | 2022-08-16 | Tdk株式会社 | 电介质组合物、电子部件及层叠电子部件 |
CN114914085B (zh) * | 2021-02-09 | 2023-10-13 | Tdk株式会社 | 电介质组合物、电子部件及层叠电子部件 |
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US10329200B2 (en) | 2019-06-25 |
EP3358039A4 (en) | 2019-05-15 |
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TW201716317A (zh) | 2017-05-16 |
EP3358039A1 (en) | 2018-08-08 |
US20180282229A1 (en) | 2018-10-04 |
TWI598290B (zh) | 2017-09-11 |
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