CN110957377B - 一种基于mos管的忆容器及其制备方法 - Google Patents
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Abstract
本发明公开了一种基于MOS管的忆容器及其制备方法。该忆容器的结构为：在衬底上依次生长有第一氧化物介质层、CuOx纳米晶层、第二氧化物介质层以及顶电极。通过在氧化物介质层中掺入具有忆阻特性的CuOx纳米晶，构成介电常数可调的复合介质层，从而使器件具有电容可调的功能。本发明的忆容器具有结构简单、环境友好、电容调节方便、可调范围大(可调率超过3000％)和可重构等优点。
Description
技术领域
本发明属于微电子器件领域，涉及一种基于MOS管忆容器及其制备方法。
背景技术
忆阻器的概念是由蔡少棠教授在1971年首先提出，直到2008年，HP实验室才首次成功制得基于双层二氧化钛薄膜的固体忆阻器。2009年，蔡少棠等在IEEE上撰文将记忆系统的概念扩展到容性和感性元件中，并详细阐述了忆容器和忆感器的特性。忆阻器、忆容器、忆感器统称为记忆元件。记忆元件凭借其纳米尺寸、低功耗、集成密度高及非线性特性，被广泛应用于存储、人工神经网络、非线性科学等领域，同时被认为是最有可能延续摩尔定律的新型元件。
忆阻器、忆容器和忆感器区别于普通的无源器件的一个特征就是其阻态、容态和感态取决于系统的历史状态，即具有记忆性。其中，忆容器根据其电容改变的物理机制不同可分为以下几种：一、精确改变器件的物理尺寸，包括微机电系统(MEMS)、纳机电系统(NEMS)和弹性电容器等，它们在无线电通信等领域有广泛应用。但此类器件设计难度大，工作方式属于耗散型。二、改变介质层的介电常数，包括利用相变、离子注入、铁电极化来调节介质的电容。2009年，T.Driscoll等人在《Science》上报道了利用VO2的金属-绝缘体转变来实现电容的连续可调和记忆，可是其同时存在工作温度区间窄、电容可调范围低和阻值改变大等问题。2010年，M.Krems等人在《Nano Letters》上发表了离子注入型的忆容器文章，它利用离子受到外场作用后穿过纳米孔洞来改变溶液的电容，但是它工作需要溶液的参与，存在与微电子器件不兼容的问题。铁电忆容系统利用铁电畴在外场作用下发生翻转实现忆容的效果，但当电场撤去后，铁电调制效果逐渐消失。因此，寻找一种制备简单、工艺兼容、电容大范围可调、可编程和重构的忆容器显得至关重要。
磁控溅射是20世纪70年代发展起来的一种溅射技术，具有高速、低温、低损伤的特点，是物理气相沉积的一种。通过靶阴极表面中引入磁场，利用磁场对带电粒子的约束来提高等离子体密度以增加溅射率。原子层化学气相沉积(ALD)技术利用气相源在衬底表面吸附或反应的自饱和性实现逐层生长，生成薄膜的厚度只与循环周期的数目有关。由于具有独特的自限制生长特点，原子层沉积成膜具有精确的厚度控制、优异的三维贴合性和大面积成膜等优点，在制备超薄薄膜、纳米结构方面独具优势。
发明内容
针对以上现有技术的缺陷，本发明提供一种基于MOS管的忆容器及其制备方法。
本发明忆容器采用的技术方案如下：
一种基于MOS管的忆容器，在衬底上依次生长有第一氧化物介质层、CuOx纳米晶层、第二氧化物介质层以及顶电极。
进一步地，所述衬底是p-型掺杂的、电阻率为1～10Ω/cm的单晶硅。
进一步地，所述第一氧化物介质层的厚度为2～10nm，第二氧化物介质层的厚度为10～20nm。
优选地，所述CuOx纳米晶层的厚度为2～10nm。
优选地，所述顶电极的结构为圆柱状点电极，直径为50～100μm，厚度为75～150nm。
本发明一种基于MOS管的忆容器的制备方法，其特征在于，步骤如下：
(1)在衬底表面生长第一氧化物介质层；
(2)在第一氧化物介质层上生长Cu薄膜，接着退火后自组装得到CuOx纳米晶层；
(3)在CuOx纳米晶层上生长第二氧化物介质层；
(4)最后在第二氧化物介质层上生长金属薄膜，作为顶电极。
进一步地，所述步骤(1)中，利用原子层薄膜沉积技术生长Al2O3的第一氧化物介质层，其中三甲基铝作为金属源，水蒸气为氧源，生长温度为250℃，生长速度为0.1nm/cycle。
进一步地，所述步骤(2)中，首先利用磁控溅射方法，在氩气气氛下，以40W功率、12nm/min的生长速率，生长Cu薄膜；接着在650～750℃下、O2的气氛中退火30～60s，自组装得到CuOx纳米晶层。
与现有技术相比，本发明具有以下有益效果：
(1)提出了一种结构简单、环境友好、基于MOS管电容器的新型忆容器，其结构为p-Si/氧化物介质层/CuOx/氧化物介质层/顶电极。MOS管电容器本身具有非线性的电容-电压特性，在氧化物介质层掺入具有忆阻特性的CuOx纳米晶后，当外加电刺激改变CuOx纳米晶的电导时，介质层的介电常数将发生变化，最终器件电容也随之变化。此时，器件具有滞后的电容-电压回线，即典型的忆容器特性。
(2)本发明忆容器具有电容调节方便、可调范围大的优点。只需施加低幅值方波电脉冲即可改变器件电容，此忆容器的电容值可以随着频率、脉冲幅值和刺激次数的增加而增加，最大可调率超过3000％。
(3)本发明忆容器具有可重构的优点。利用电脉冲改变其电容后，只需要施加相反极性的电脉冲即可使器件电容回到初始状态。
(4)采用磁控溅射法制备的Cu薄膜，具有纯度高、致密性好、成膜均匀与氧化物薄膜结合均匀的优点。此外，相比其他制备技术，磁控溅射还具备操作简便、可重复性好、成本较低的特点。
附图说明
图1是本发明忆容器的结构示意图。
图2是忆容器在不同频率下的电荷-电压滞后曲线。其中x轴表示施加在顶电极上的电压，y轴表示MOS管电容器两端的电荷，不同曲线分别代表不同的扫描频率。
图3是电脉冲刺激次数对忆容器电容的影响。其中x轴是扫描频率，y轴是0V偏压下的电容值，不同曲线代表不同的电脉冲刺激次数。
图4是忆容器的电容可调率测试图。施加不同的电脉冲以调制器件电容，其中x轴代表施加脉冲的幅值，y轴代表器件电容。脉冲宽度保持150ms，幅值的变化规律为0V→8V→-8V→0V，变化梯度为0.5V。每施加一次脉冲后，在0V偏压、1M Hz的条件下读取器件电容。
图5是忆容器的可重构性测试图，其中x轴是扫描频率，y轴是0V偏压下的电容值。三条曲线分别代表初始状态器件电容、施加正脉冲后增大的器件电容、接着施加负脉冲恢复到初始态的器件电容。
具体实施方式
本发明忆容器的结构为：p-Si/氧化物介质层/CuOx/氧化物介质层/顶电极。具有单一氧化物介质层的MOS管电容器本身具有非线性的电容-电压特性，本发明在氧化物层中掺入CuOx纳米晶，构成复合介质层。这样，器件将表现出滞后的电容-电压回线，即典型的忆容器特性。这是由于CuOx纳米晶具有忆阻特性，外加电刺激可以改变CuOx纳米晶和介质层的电导；根据Maxwell-Wagner模型，介质层的介电常数是其电导的函数。换言之，介质层介电常数和器件电容可由外加电脉冲调制。
该忆容器各层的生长方法如下：
(1)选用电阻率为1～10Ω/cm的p型掺杂的单晶硅(p-Si)作为衬底。
(2)利用化学气相沉积、磁控溅射、原子层沉积技术或电子束蒸镀等方法，在衬底表面生长2～10nm厚的第一氧化物介质层(HfO2、Al2O3、SiO2)。该介质层除作为复合电介质(包括第一氧化物介质层和第二氧化物介质层)的一部分外，由于该层厚度极小，可以将第一氧化物介质层视为隧穿层，硅衬底电子在外加垂直电场的作用下，可以越过势垒隧穿到CuOx纳米晶层，被CuOx层中的缺陷俘获。此时，在衬底和第一氧化物介质层界面处，空穴将进一步累积，从而提高器件电容的可调范围。
(3)可利用磁控溅射或分子束外延技术，在第一氧化物介质层上生长2～10nm的Cu薄膜，接着在650～750℃下和O2的气氛中退火30～60s，自组装得到CuOx纳米晶层。该厚度的CuOx层具有显著且稳定的忆阻特性，通过施加电脉冲可以显著改变其电阻，从而提高器件的电容可调率。
(4)第二氧化物介质层可为薄层的氧化物，如HfO2、Al2O3、SiO2等。可利用化学气相沉积、原子层沉积技术或电子束蒸镀等方法，在CuOx纳米晶层上生长10～20nm的氧化物薄膜，从而完成复合电介质层的构建。第二氧化物介质层除作为复合电介质的一部分外，由于该层厚度较大，可以将该氧化物介质层视为阻挡层，它的存在可以阻挡电子进一步向电极方向运动，确保电子被CuOx层的缺陷俘获。
(5)顶电极可选用电阻率较低，且能够与介质层实现欧姆接触的金属薄膜，如Au、Pt、Cu等，其厚度应在75～150nm范围，可通过磁控溅射、电子束蒸镀、脉冲激光沉积等方式实现薄膜生长。
由上述方法制备的MOS忆容器件，其结构如图1所示。
实施例
本实施例给出一种忆容器件的制备过程，具体如下：
1、将p-Si衬底分别用适量的丙酮、乙醇、去离子水超声清洗10分钟，清洗掉Si表面的有机物等杂质。然后再将衬底放入HF:H2O＝1:10的氢氟酸溶液中浸泡30s，去除表面氧化物，再用去离子水超声清洗5分钟，洗掉残余的氢氟酸，用高纯氮气吹干后放入原子层沉积腔体内沉积薄膜。
2、采用原子层沉积技术在衬底上沉积厚度为3nm的Al2O3作为介质层。在沉积过程中用三甲基铝(Al(CH3)3)作为金属源，水蒸气为氧源，生长温度为250℃，生长速度为0.1nm/cycle，共生长30个循环。
3、接着将步骤2得到的样品放入磁控溅射生长腔内，在样品表面沉积约5nm厚的金属Cu薄膜，生长功率为40W，气氛为氮气(4Pa)，生长速率为12nm/min。
4、生长完Cu薄膜后，将样品放入快速退火炉中退火，使Cu膜氧化并团聚成CuOx纳米晶。退火条件是700℃，氧气气氛，退火时间40s。
5、将退火后的样品再用ALD沉积12nm厚的Al2O3介质层，生长条件与步骤2所述相同，循环次数为120次。
6、接着在样品表面用磁控溅射生长约100nm的铂金作为上电极，生长功率为15W，气氛为氩气(2Pa)，生长速率为9nm/min。
7、最后，在Si衬底上涂一层导电银胶作为底电极。
制备完成后进行测量，实验中忆容器件的电荷-电压滞后曲线以及电容-频率变化曲线均使用Keithley 4200半导体参数分析仪完成。
电容可调行为的测试方法为：用Keithley 4200首先测得初始状态下忆容器的电容-频率曲线，再用Keithley 4200中的PMU模块在上电极上施加10个脉冲，脉冲幅值为8V，脉冲宽度为0.15s，测得器件刺激后的电容-频率曲线，接着给忆容器施加若干-8V 0.1s的脉冲，将其电容值调至初始状态。20个脉冲刺激后的电容-频率曲线同样按照此步骤进行。
如图2，在频率分别为100k、1M Hz的条件下，测得器件在+8V和-8V之间的电容-电压回线，利用电容定义式计算后，得到忆容器的电荷-电压的滞后回线，该回线的存在证明的器件具有忆容特性。
如图3，相比初始状态，施加正脉冲后，器件电容显著增大。器件电容的随施加脉冲次数的增大而增大，随频率的增大而减小，由此实现了对器件电容的调制。
电容可调率的测试方法：分别测得特定的频率、脉冲幅值、脉冲次数刺激后的忆容器的电容值C，已知初始转态下1MHz的电容值为C0，得到忆容器的电容可调率为T＝(C-C0)/C0×100％，最终做出电容可调率相图。本实施例的忆容器的电容值可以随着频率、脉冲幅值和刺激次数的增加而增加。如图4，施加正脉冲可使器件电容增大，施加负脉冲则会使器件电容降低。当脉冲幅值处于2～4V，-2～-4V范围，器件可调率的变化最为显著。在施加+8V、150ms的脉冲后，器件电容可调率超过了3000％。
电容可重构性的测试方法：首先测得初始状态下的电容-频率曲线，接着在上电极上施加+8V 0.15s的电压脉冲，测得刺激后的电容-频率曲线，然后再在上电极上施加-8V 3μs的电压脉冲，再次测量忆容器的电容-频率曲线。如图5，对处于初始态的器件施加正脉冲，器件电容在全频率范围下，特别是低频下显著增大，再施加合适的负脉冲，器件电容回到初始状态，由此完成了对器件电容的重构。
Claims (4)
1.一种基于MOS管的忆容器的制备方法，其特征在于，步骤如下：
(1)在衬底表面生长第一氧化物介质层；
(2)在第一氧化物介质层上生长Cu薄膜，接着退火后自组装得到CuOx纳米晶层，具体步骤为：首先利用磁控溅射方法，在氩气气氛下，以40W功率、12nm/min的生长速率，生长Cu薄膜；接着在650～750℃下、O2的气氛中退火30～60s，自组装得到CuOx纳米晶层；
(3)在CuOx纳米晶层上生长第二氧化物介质层；
(4)最后在第二氧化物介质层上生长金属薄膜，作为顶电极。
2.根据权利要求1所述的一种基于MOS管的忆容器的制备方法，其特征在于，所述步骤(1)中，利用原子层薄膜沉积技术生长Al2O3的第一氧化物介质层，其中三甲基铝作为金属源，水蒸气为氧源，生长温度为250℃，生长速度为0.1nm/cycle。
3.根据权利要求1所述的一种基于MOS管的忆容器的制备方法，其特征在于，所述步骤(3)中，第二氧化物介质层的厚度为10～20nm。
4.根据权利要求1所述的一种基于MOS管的忆容器的制备方法，其特征在于，所述步骤(4)中，顶电极的厚度为75～150nm。
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