CN111180540A - 基于单晶硅纳米膜/石墨烯的柔性光电探测器及制备方法 - Google Patents

基于单晶硅纳米膜/石墨烯的柔性光电探测器及制备方法 Download PDF

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CN111180540A
CN111180540A CN201911405518.2A CN201911405518A CN111180540A CN 111180540 A CN111180540 A CN 111180540A CN 201911405518 A CN201911405518 A CN 201911405518A CN 111180540 A CN111180540 A CN 111180540A
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吕朝锋
陆明
徐杨
茅仁伟
刘粒祥
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Zhejiang University ZJU
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Abstract

本发明公开一种基于单晶硅纳米膜/石墨烯的柔性光电探测器及制备方法，该光电探测器由聚酰亚胺衬底、金属互连导线、单晶硅纳米薄膜、单原子层石墨烯以及顶层聚酰亚胺组成。本发明基于体硅/石墨烯肖特基异质结光电探测器优异性能的基础上，将体硅减薄到纳米级尺度，使原本大而坚硬的固体硅变得薄而柔且可实现较大程度上的弯曲，经柔性封装材料聚酰亚胺封装后，在保留体硅/石墨烯异质结优异光电探测性能的基础上，还具有了超薄、柔性的优点，结合聚酰亚胺的高绝缘性和良好的生物相容性，大大拓宽了硅/石墨烯异质结光电探测器的应用领域，尤其是生物医学领域、可穿戴电子设备领域等。

Description

基于单晶硅纳米膜/石墨烯的柔性光电探测器及制备方法
技术领域
本发明涉及光电探测器领域，具体涉及基于单晶硅纳米膜/石墨烯的柔性光电探测器及制备方法。
背景技术
光电传感器的基本原理以光电效应为基础，当光照射在某些物质上时，光子的能量会传递给电子，使电子所处的状态发生改变，从而使该物质的电学特性发生相应改变，达到将光信号转换为电信号的一种器件。光电探测器在通信、医疗卫生、计算机技术、空间技术等领域有着广泛的应用。
单晶硅/石墨烯肖特基异质结光电探测器具有高灵敏度、高光学响应、响应速度快等优点，在高速信号调制、微弱信号探测等方面具有重要应用。传统单晶硅/石墨烯肖特基异质结光电探测器性能优异，但无法做到柔性化，其应用领域受到极大限制，尤其在生物医学领域，可穿戴柔性电子器件正展现出蓬勃的活力；而其它类型柔性光电探测器，一方面探测性能不如硅基光电探测器，另一方面制备成本较高，不能与现有集成电路工艺相兼容。
发明内容
针对现有技术的不足，本发明提供一种基于单晶硅纳米膜/石墨烯的柔性光电探测器及制备方法，该光电探测器肖特基结感光部位可以做到较大角度弯曲，整体器件具有性能优异、超薄、柔性化及良好的生物兼容性等优点。具体技术方案如下：
一种基于单晶硅纳米膜/石墨烯的柔性光电探测器，它由柔性衬底、两根金属互连导线、单晶硅纳米薄膜、石墨烯以及顶层柔性封装层组成，其中所述的一根金属互连导线与单晶硅纳米薄膜接触处形成一个金属接触电极，所述的另一根金属互连导线与石墨烯形成另一个金属接触电极，所述的纳米薄膜与石墨烯有一交叠区域，形成单晶硅/石墨烯肖特基异质结；肖特基异质结处产生的信号分别通过所述的两个金属接触电极引出；所述的金属互连导线末端的顶层柔性封装层被刻蚀掉，裸露出金属互连导线，将信号与外接电路相连。
进一步地，所述单晶硅纳米薄膜厚度为100nm～300nm，所述的金属互连导线的厚度为30nm～100nm。
进一步地，所述单晶硅纳米薄膜从绝缘体上硅剥离而得，且为多孔结构。
进一步地，所述单晶硅纳米薄膜通过湿法转印的方法转印到所述的柔性衬底上的金属接触电极处。
进一步地，所述的柔性衬底和顶层柔性封装层均由聚酰亚胺制成。
一种如所述的柔性光电探测器的制备方法，该方法具体包括如下步骤：
S1:在基底上旋涂柔性衬底材料，使其固化，形成柔性衬底；
S2：在所述的柔性衬底光刻金属互连导线图案；
S3：电子束蒸发金属，形成金属互连导线；
S4：在衬底指定位置通过湿法转印的方法转印大规模单晶硅纳米薄膜；
S5：光刻单晶硅纳米薄膜图案，刻蚀完全裸露的单晶硅，得到特定位置处特定尺寸的单晶硅纳米薄膜；
S6：指定位置转印石墨烯，光刻石墨烯图案；
S7：完全刻蚀裸露的石墨烯，得到特定位置处特定尺寸的单原子层石墨烯；
S8：旋涂柔性封装层材料，使其固化，对制作好的器件进行封装；
S9：光刻所述的柔性封装层材料刻蚀阻挡层图案，电子束蒸发金属，形成刻蚀阻挡层图案；
S10；刻蚀未被刻蚀阻挡层遮挡的柔性封装层材料，把刻蚀好的器件放入刻蚀液中，刻蚀掉底部的基板，得到柔性光电探测器。
进一步地，所述的柔性衬底材料为聚酰亚胺，所述的基板为玻璃。
进一步地，所述的金属互连导线由Cr和Au组成，所述的S3中电子束蒸发时，先蒸Cr,后蒸Au。
进一步地，所述的S9中的刻蚀阻挡层由Al制成。
进一步地，所述的刻蚀液为缓冲氧化物刻蚀液。
本发明的有益效果如下：
本发明提出的基于单晶硅纳米膜/石墨烯的柔性光电探测器，该光电探测器肖特基结感光部位可以做到较大角度弯曲，既保证了单晶硅/石墨烯肖特基异质结光电探测器的优异性能，同时由于采用的是单晶硅纳米薄膜，使器件具有良好的柔性，本发明的光电探测器性能优异、超薄，具有良好的生物兼容性，大大扩充了光电探测器的应用领域，尤其是生物医学领域。
本发明提出的基于单晶硅纳米膜/石墨烯的柔性光电探测器制备方法，该方法与传统硅基电子技术工艺相兼容，且能制备出柔性光电探测器，能够将传统硅基电子技术与柔性电子技术相融合，为将传统硅基电子技术与柔性电子技术相结合提供了一种新思路。
附图说明
图1是器件的三维透视图。
图2是器件未旋涂顶层聚酰亚胺的前视图。
图3是本发明制备方法的工艺流程图。
图4是器件实物图。
图中：1、聚酰亚胺衬底，2、金属互连导线，3、单晶硅纳米薄膜，4、单原子层石墨烯，5、聚酰亚胺封装层，6、单晶硅与金属接触电极，7、石墨烯与金属接触电极，8、刻蚀掉顶层聚酰亚胺封装层的金属互连导线末端，9、器件实物。
具体实施方式
下面根据附图和优选实施例详细描述本发明，本发明的目的和效果将变得更加明白，应当理解，此处所描述的具体实施例仅仅用以解释本发明，并不用于限定本发明。
如图1-2所示，本发明提出的基于单晶硅纳米薄膜/石墨烯异质结超薄、柔性化光电探测器，包括：聚酰亚胺衬底1、金属互连导线2、单晶硅纳米薄膜3、单原子层石墨烯4以及聚酰亚胺封装层5。
单晶硅纳米薄膜3与单原子层石墨烯4有一交叠区域6，形成单晶硅/石墨烯肖特基异质结。肖特基异质结处产生的信号分别通过单晶硅与其中一根所述的金属互连导线形成的金属接触电极6及石墨烯与另一根金属互连导线形成的金属接触电极7引出。整个光电传感器由聚酰亚胺衬底1及顶层聚酰亚胺5封装而成，使光电传感器与外界环境绝缘，可以在潮湿或液体环境中工作。金属互连导线末端8的聚酰亚胺封装层被刻蚀掉，裸露出金属互连导线，通过导电纸将信号与外接电路相连。整个光电传感器9组成部位均具有一定的柔性，这是一个真柔性化光电传感器。
单晶硅的厚度减薄到纳米等级之后，其可弯曲半径变得非常小，表现出良好的柔性性能。
单原子层石墨烯4通过CVD方法在铜箔衬底上制备获得，具有高透光率和宽光谱吸收的优异性能，与单晶硅表面接触形成超浅肖特基异质结。
聚酰亚胺具有极佳的柔性、高绝缘性和良好的生物相容性，因此，本发明选用聚酰亚胺来制作衬底和封装层。
在本实施例，单晶硅纳米薄膜通过湿法转印的方法转印到所述的柔性衬底上的金属接触电极处。所述单晶硅纳米薄膜从绝缘体上硅剥离而得，且为多孔结构。
为了提高金属互连导线的导电性，以及保证单晶硅纳米薄膜和石墨烯在与金属互连导线接触时的完整性，该接触电极的厚度不能太厚也不能太薄，优选30nm～100nm。
为了提高金属互连导线与衬底间的粘附，同时避免金属互连导线在器件从基板上剥离下来时不被腐蚀液腐蚀，所述金属互连导线先沉积金属Cr增加粘附性，后沉积金属金避免被腐蚀液腐蚀。
为了保证单晶硅薄膜的柔性和可获得性，所述单晶硅纳米薄膜厚度优选100nm～300nm。
本发明还提供了一种基于单晶硅纳米薄膜/石墨烯异质结超薄、柔性化光电探测器的制作方法和工艺，如图3所示，首先准备玻璃基底，采用旋涂的方法在玻璃基板上旋涂固化一层聚酰亚胺衬底，在该衬底上通过光刻和电子束蒸发蒸镀一层金属互连导线，再通过湿法转印的方式将单晶硅纳米薄膜和单原子层石墨烯转印至衬底对应电极位置处，分别刻蚀成形，形成肖特基结感光区域，再通过光刻电子束蒸发蒸镀一层铝金属阻挡层，刻蚀掉不需要的聚酰亚胺和金属互连导线末端顶层的聚酰亚胺，使电极裸露，最终通过缓冲氧化物刻蚀液刻蚀掉聚酰亚胺衬底下方的玻璃基板剥离出单个的超薄柔性光电探测器。
所述制作工艺按照如下步骤：
S1：制备聚酰亚胺衬底。在直径为10厘米，厚度为1.1毫米的玻璃基片上，旋涂一层聚酰亚胺薄膜，旋涂工艺的参数为：500r/min 10s,2000r/min 60s。旋涂完成后放置在加热板上加热，经过加热固化形成聚酰亚胺衬底，加热工艺参数为80℃1小时，120℃1小时，170℃1小时，230℃1小时。
S2：在聚酰亚胺衬底上光刻金属互连导线图案，显影。
S3：显影好的衬底放入电子束蒸发设备中蒸镀一层金属，电子束蒸发工艺为Cr/Au5nm/60nm。将蒸镀好金属的衬底依次放入丙酮、异丙醇溶液中洗去剩余的光刻胶，形成金属互连导线，再放入去离子水中清洗干净。
S4:转印单晶硅纳米薄膜至聚酰亚胺衬底上一侧电极处。将从SOI上剥离下来的漂浮在水面上的方块单晶硅纳米薄膜(优选的，尺寸为5mm*5mm)，通过湿法转印的方式，用聚酰亚胺衬底把单晶硅纳米薄膜从水中定点捞起，置于一侧电极处。
1)在SOI顶层硅上光刻刻蚀边长为5微米、间距为400微米的方形孔阵列，该方形孔阵列外围刻蚀一边宽为20微米、边长为5毫米的方形沟槽，方形孔阵列及方形沟槽都刻蚀到SOI埋氧层部位。
2)将刻蚀好的SOI放入缓冲氧化物刻蚀液中浸泡，待埋氧层腐蚀完后，轻轻晃动液体，单晶硅纳米薄膜会悬浮于液体表面，用载玻片捞起，转印至去离子水中，浸泡一段时间，洗去缓冲氧化物刻蚀液。(注意：该步骤涉及到缓冲氧化物刻蚀液，较为危险，操作时应做好安全防护措施)。
3)用附着在玻璃基底上的聚酰亚胺衬底去捞悬浮在去离子水表面的单晶硅纳米薄膜，此时由于聚酰亚胺衬底上已蒸镀上一层金属互连导线，而单晶硅纳米薄膜的尺寸也比较大(5毫米*5毫米)，故可以通过肉眼分辨的方式将单晶硅纳米薄膜定点转印到电极处，而实际所需的用于形成光电探测器的单晶硅纳米薄膜尺寸远远小于方块尺寸，可以通过刻蚀的方式把其余地方的单晶硅纳米薄膜刻蚀掉。
S5:对于转印至衬底上的单晶硅纳米薄膜进行光刻、显影，裸露出所需区域外的单晶硅纳米薄膜，将样品放入ICP刻蚀机中，刻蚀掉所需区域外的单晶硅纳米薄膜。
S6:转印单原子层石墨烯至聚酰亚胺衬底上另一侧电极处并与之前转印至衬底上并经过刻蚀后剩余的单晶硅纳米薄膜有一定的交叠区域。将CVD生长在铜箔衬底上的单原子层石墨烯旋涂PMMA支撑层后，刻蚀掉铜箔衬底，通过湿法转印的方法运用前述聚酰亚胺衬底把单原子层石墨烯从水中定点捞起，置于另一侧电极处，并与前述刻蚀后单晶硅纳米薄膜有一定交叠区域。
1)在附有CVD生长石墨烯的铜箔表面旋涂一层PMMA支撑层，加热固化。
2)将覆有PMMA支撑层的铜箔放入五水硫酸铜与盐酸配置的溶液中，刻蚀掉铜箔衬底。
3)铜箔衬底刻蚀完全后，单原子层石墨烯附着在PMMA支撑层表面，漂在溶液上。
4)用载玻片把附有石墨烯的PMMA捞起放入去离子水中静置一段时间，再捞起放入新的去离子水中，反复几次，把石墨烯漂洗干净。
5)用附着在玻璃基底上的聚酰亚胺衬底将石墨烯定点转印到另一侧电极处。
S7:刻蚀所需区域外的单原子层石墨烯。将转印至衬底上的石墨烯表面的PMMA支撑层洗去，之后进行光刻、显影，使所需区域外的石墨烯裸露出来，用ICP刻蚀机把裸露出的单原子层石墨烯刻蚀掉。
由于此时聚酰亚胺衬底上已有光刻对准标记，可以再进行一步光刻淀积金属互联导线工艺，增强单晶硅纳米薄膜与金属电极以及单原子层石墨烯与金属互连导线之间的接触。然后进行S8。
S8:在聚酰亚胺衬底表面再旋涂一层聚酰亚胺，加热固化，把制作好的光电传感器封装起来，并刻蚀掉互连导线末端顶层聚酰亚胺，裸露出导线，以便与外部电路互连。
S9：光刻所述的柔性封装层材料刻蚀阻挡层图案，电子束蒸发金属，形成刻蚀阻挡层图案；
S10；刻蚀未被刻蚀阻挡层遮挡的柔性封装层材料，把刻蚀好的器件放入刻蚀液中，刻蚀掉底部的基板，得到柔性光电探测器。
1)在制作好光电探测器的聚酰亚胺衬底表面，再次旋涂一层聚酰亚胺，加热固化，对器件进行封装。
2)光刻聚酰亚胺刻蚀阻挡层图案，显影。
3)电子束蒸镀铝金属阻挡层，洗去光刻胶，未被光刻胶覆盖的衬底区域会留下一层金属铝薄膜刻蚀阻挡层。
4)ICP刻蚀未被铝金属阻挡层遮挡的聚酰亚胺，形成器件形状。此步骤会刻蚀掉互连导线末端顶层的聚酰亚胺，使原本完全封装的器件在互连导线末端可以与外接电路互连而不破坏光电传感器肖特基结感光区域的封装层，金属互连导线下方的衬底聚酰亚胺由于有互连导线作为阻挡层，不会被刻蚀掉，保证衬底聚酰亚胺完整性。
5)把刻蚀好的器件放入缓冲氧化物刻蚀液中，刻蚀液会从刻蚀掉聚酰亚胺的位置往内部扩散，刻蚀掉聚酰亚胺下方的玻璃基板，同时也会腐蚀掉蒸镀在聚酰亚胺表面的金属铝阻挡层，使得器件可以重新透光，接受光信号。该步骤得到独立的柔性、超薄光电传感器。
6)将剥离下来的器件在清水中反复漂洗，清洗干净，用滤纸把器件捞起来，放在热板上加热烘干，用导电纸与裸露电极互连，引出信号。
如图4所示器件实物，为根据本发明具体实施方式制备而成，其各结构材料及尺寸为，聚酰亚胺衬底及聚酰亚胺封装层厚度均3微米，金属互连导线材料为铬、金，铬厚度5纳米，金厚度60纳米，单晶硅纳米薄膜厚度220纳米，刻蚀后长度2000微米，宽度1000微米，单晶硅纳米薄膜与其中一个金属导线接触面积为1000微米*1000微米，刻蚀后石墨烯长度2000微米，宽度1000微米，石墨烯与金属电极接触面积为1000微米*1000微米，单晶硅纳米薄膜与石墨烯接触面积为1000微米*1000微米。
本领域普通技术人员可以理解，以上所述仅为发明的优选实例而已，并不用于限制发明，尽管参照前述实例对发明进行了详细的说明，对于本领域的技术人员来说，其依然可以对前述各实例记载的技术方案进行修改，或者对其中部分技术特征进行等同替换。凡在发明的精神和原则之内，所做的修改、等同替换等均应包含在发明的保护范围之内。

Claims (10)

1.一种基于单晶硅纳米膜/石墨烯的柔性光电探测器，其特征在于，它由柔性衬底、两根金属互连导线、单晶硅纳米薄膜、石墨烯以及顶层柔性封装层组成，其中所述的一根金属互连导线与单晶硅纳米薄膜接触处形成一个金属接触电极，所述的另一根金属互连导线与石墨烯形成另一个金属接触电极，所述的纳米薄膜与石墨烯有一交叠区域，形成单晶硅/石墨烯肖特基异质结；肖特基异质结处产生的信号分别通过所述的两个金属接触电极引出；所述的金属互连导线末端的顶层柔性封装层被刻蚀掉，裸露出金属互连导线，将信号与外接电路相连。
2.根据权利要求1所述的基于单晶硅纳米膜/石墨烯的柔性光电探测器，其特征在于，所述单晶硅纳米薄膜厚度为100nm～300nm，所述的金属接触电极的厚度为30nm～100nm。
3.根据权利要求1所述的基于单晶硅纳米膜/石墨烯的柔性光电探测器，其特征在于，所述单晶硅纳米薄膜从绝缘体上硅剥离而得，且为多孔结构。
4.根据权利要求1所述的基于单晶硅纳米膜/石墨烯的柔性光电探测器，其特征在于，所述单晶硅纳米薄膜通过湿法转印的方法转印到所述的柔性衬底上的金属接触电极处。
5.根据权利要求1所述的基于单晶硅纳米膜/石墨烯的柔性光电探测器，其特征在于，所述的柔性衬底和顶层柔性封装层均由聚酰亚胺制成。
6.一种如权利要求1所述的柔性光电探测器的制备方法，其特征在于，该方法具体包括如下步骤：
S1:在基底上旋涂柔性衬底材料，使其固化，形成柔性衬底；
S2：在所述的柔性衬底光刻显影金属互连导线图案；
S3：电子束蒸发金属，洗去光刻胶，形成金属互连导线；
S4：通过湿法转印的方法转印单晶硅纳米薄膜至衬底金属互连导线一端；
S5：光刻显影单晶硅纳米薄膜图案，刻蚀完全裸露的单晶硅，得到特定位置处特定尺寸的单晶硅纳米薄膜；
S6：转印石墨烯至衬底另一金属互连导线一端，光刻显影石墨烯图案；
S7：完全刻蚀裸露的石墨烯，得到特定位置处特定尺寸的石墨烯；
S8：旋涂柔性封装层材料，使其固化，对制作好的器件进行封装；
S9：光刻显影所述的柔性衬底及柔性封装层材料刻蚀阻挡层图案，电子束蒸发金属，形成刻蚀阻挡层图案；
S10；刻蚀未被刻蚀阻挡层遮挡的柔性衬底及柔性封装层材料，把刻蚀好的器件放入刻蚀液中，刻蚀掉底部的基板，得到柔性光电探测器。
7.根据权利要求6所述的柔性光电探测器的制备方法，其特征在于，所述的柔性衬底及柔性封装层材料为聚酰亚胺，所述的基板为玻璃。
8.根据权利要求6所述的柔性光电探测器的制备方法，其特征在于，所述的金属互连导线由Cr和Au组成，所述的S3中电子束蒸发时，先蒸Cr,后蒸Au。
9.根据权利要求6所述的柔性光电探测器的制备方法，其特征在于，所述的S9中的刻蚀阻挡层由Al制成。
10.根据权利要求6所述的柔性光电探测器的制备方法，其特征在于，所述的刻蚀液为缓冲氧化物刻蚀液。
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