CN108493096B - 一种退火处理形成电荷存储结构的方法 - Google Patents

一种退火处理形成电荷存储结构的方法 Download PDF

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CN108493096B
CN108493096B CN201810212709.6A CN201810212709A CN108493096B CN 108493096 B CN108493096 B CN 108493096B CN 201810212709 A CN201810212709 A CN 201810212709A CN 108493096 B CN108493096 B CN 108493096B
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汤振杰
李�荣
胡丹
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Abstract

本发明公开了一种退火处理形成电荷存储结构的方法，通过退火过程，借助单层多组元金属氧化物(M)x(N)1‑x薄膜退火过程中低结晶温度M析晶、扩散和重新分布的特点，自发形成富N的(M)x(N)1‑x隧穿层/富M的(M)x(N)1‑x存储层/富N的(M)x(N)1‑x阻挡层电荷存储结构，其中M可在ZrO2、HfO2、La2O3、TiO2中任选一种，N可在SiO2、Al2O3中任选一种。

Description

一种退火处理形成电荷存储结构的方法
技术领域
本发明属微电子器件及其材料领域，涉及一种利用退火处理形成电荷存储结构的方法。
背景技术
随着信息社会的不断进步，非易失性半导体存储器获得了前所未有的发展。在非易失性存储器件家族当中，硅-氧化物-氮化物-氧化物-多晶硅(SONOS)型电荷陷阱存储器件以其稳定性高、与半导体工艺兼容性好等优点成为一种极具应用前景的存储结构，其中紧邻硅(Si)衬底的氧化物(SiO2)隧穿层、氮化物(Si3N4)存储层、以及紧挨着多晶硅电极的氧化物(SiO2)阻挡层构成典型的三明治电荷存储结构。器件在编程操作下，电荷穿过隧穿层，进入到存储层，被存储层中的缺陷俘获，从而达到信息存储的目的，其中阻挡层和隧穿层的存在，抑制了存储电荷在数据保持状态下，向衬底和电极方向的泄漏。
对于传统的SONOS型电荷存储器件，通常利用化学气相沉积、物理溅射等方法在衬底材料表面顺序生长隧穿层、存储层、和阻挡层形成电荷存储结构，器件制备过程比较复杂。基于简化非易失性电荷存储器件制备过程的考虑，我们发明了一种退火处理单层多组元金属氧化物薄膜工艺，借助多组元氧化物薄膜结晶过程组分重新分布机理，自发形成具有三明治电荷存储结构。
发明内容
本发明提供了一种退火处理单层多组元金属氧化物薄膜工艺，形成电荷存储结构的方法，操作简单。
所述退火处理形成电荷存储结构的方法具体过程如下：
a)将硅衬底置于丙酮中，超声清洗1分钟，去除衬底表面杂质，然后将衬底置于氢氟酸稀溶液中，去除硅衬底表面的氧化物，然后将硅衬底放置在脉冲激光沉积系统腔内的衬底台上，将多组元金属氧化物(M)x(N)1-x和铝(Al)靶材置于靶材底盘上，其中M可在ZrO2、HfO2、 La2O3、TiO2中任选一种，N可在SiO2、Al2O3中任选一种，x在0.5-0.8范围内取值，沉积腔内压强为1×10-5Pa-5×10-5Pa；
b)利用脉冲激光沉积系统在硅衬底表面沉积一层厚度为20-30nm的(M)x(N)1-x薄膜，如图1(a)所示；
c)将衬底台温度升高到850℃，沉积的(M)x(N)1-x薄膜在850℃下，退火处理1小时，使 (M)x(N)1-x薄膜中发生相分离反应，结晶温度较低的M相趋向在(M)x(N)1-x薄膜中间部位析出，随着退火过程的进行，组分不断扩散和重新分布，晶粒逐渐粗化和长大，造成(M)x(N)1-x薄膜中间部位M组元较多，N组元较少，形成富M的(M)x(N)1-x，而(M)x(N)1-x薄膜两侧M组元较少，N组元较多，形成富N的(M)x(N)1-x，单层(M)x(N)1-x薄膜在退火过程中自发形成三明治电荷存储结构，其中靠近硅衬底的富N的(M)x(N)1-x层作为隧穿层，富M的(M)x(N)1-x层作为电荷存储层，远离硅衬底的富N的(M)x(N)1-x层作为阻挡层，如图1(b)所示；
d)利用脉冲激光沉积系统在(M)x(N)1-x薄膜表面沉积一层100-200nm的Al金属作为电极，如图1(c)所示；
上述方法的原理是基于单层(M)x(N)1-x薄膜退火处理过程的组分重新分布，由于M较N 具有更低的结晶温度，在退火过程中析出，并随着退火时间延长，M向薄膜中间部位扩散， N向薄膜两边扩散，导致M晶粒在薄膜中间部位聚集并长大。因此，单层(M)x(N)1-x薄膜在退火处理过程中会自发形成富N的(M)x(N)1-x/富M的(M)x(N)1-x/富N的(M)x(N)1-x三明治电荷存储结构。图2(a)为未退火处理的单层(M)x(N)1-x薄膜能带图，由于薄膜组分均匀，因此薄膜能带一致。经过退火处理，薄膜组分扩散和重新分布，M趋向聚集于薄膜中间，而N趋向聚集于薄膜两侧。M较N具有更小的禁带宽度，所以M含量越多，禁带宽度越小，N含量越多，禁带宽度越大，如图2(b)所示。
优选(ZrO2)0.8(Al2O3)0.2薄膜，厚度为20nm，依据上述方法得到的结构，可用高分辨透射电子显微截面图表征，如图3所示：
从图3(a)中可以看出，未实施退火处理的(ZrO2)0.8(Al2O3)0.2为单层结构，而经过850℃， 1小时的退火处理后(图3(b))，低结晶温度的ZrO2趋于在接近薄膜中间部位结晶长大，形成富ZrO2的(ZrO2)x(Al2O3)1-x，厚度约为10nm，由于ZrO2大部分扩散到薄膜中间部位结晶，薄膜两侧形成富Al2O3的(ZrO2)x(Al2O3)1-x。通过退火处理单层(ZrO2)0.8(Al2O3)0.2薄膜，利用退火过程中组分的扩散和重新分布，实现了典型的三明治电荷存储结构，其中薄膜中间富ZrO2的(ZrO2)x(Al2O3)1-x薄膜层对应电荷存储结构的存储层，富Al2O3的(ZrO2)x(Al2O3)1-x薄膜层分别对应隧穿层和阻挡层。
上述方法所得电荷存储结构的存储性能可用不同栅极扫描电压下，电容-电压变化曲线表征，如图4所示：
从图中可以看出，未经过退火处理的薄膜，在不同栅极扫描电压下，没有表现出电容- 电压存储窗口，表明没有电荷存储性能，如图4(a)所示；而经过退火处理的薄膜，在±6V和±8V的栅极扫描电压下，分别具有2V和4V的存储窗口，表明该结构具有电荷存储性能。这主要是因为(ZrO2)0.8(Al2O3)0.2薄膜经过退火处理，薄膜组分重新分布，自发形成典型的三明治电荷存储结构。当Al电极施加正向电压时，电场指向硅衬底方向，衬底当中的电子在电场力的作用下穿过富Al2O3的(ZrO2)x(Al2O3)1-x隧穿层进入富ZrO2的(ZrO2)x(Al2O3)1-x存储层，被存储层中的缺陷俘获，引起平带电压向正向的偏移；当Al电极施加负向电压时，电场指向Al电极，富ZrO2的(ZrO2)x(Al2O3)1-x存储层俘获的电荷在电场力的作用下，穿过富Al2O3的 (ZrO2)x(Al2O3)1-x隧穿层回到衬底，引起平带电压向负向的偏移，从而表现出电容-电压存储窗口。
附图说明
图1：(a)利用脉冲激光沉积系统在硅衬底表面沉积(M)x(N)1-x薄膜；(b)退火处理后由于组分扩散和重新分布，(M)x(N)1-x薄膜自发形成三明治电荷存储结构；(c)利用脉冲激光系统沉积 Al电极。
图2：单层(M)x(N)1-x薄膜退火处理前后能带排列示意图，(a)退火处理前，(b)退火处理后。
图3：单层(ZrO2)0.8(Al2O3)0.2薄膜退火处理前后薄膜的高分辨透射电子显微结构截面图，(a) 退火处理前，(b)退火处理后。
图4：单层(ZrO2)0.8(Al2O3)0.2薄膜退火处理前后的电荷存储性能，(a)退火处理前，(b)退火处理后。
具体实施方式
实施例1：单层(ZrO2)0.8(Al2O3)0.2薄膜制备过程如下：
a)将硅衬底置于丙酮中，超声清洗1分钟，去除衬底表面杂质，然后将衬底置于氢氟酸稀溶液中，去除硅衬底表面的氧化物，然后将硅衬底放置在脉冲激光沉积系统腔内的衬底台上，将多组元金属氧化物(ZrO2)0.8(Al2O3)0.2和铝(Al)靶材置于靶材底盘上，沉积腔内压强为1 ×10-5Pa；
b)利用脉冲激光沉积系统在Si衬底表面沉积一层厚度为20nm的(ZrO2)0.8(Al2O3)0.2薄膜；
c)利用脉冲激光沉积系统在(ZrO2)0.8(Al2O3)0.2薄膜表面沉积一层100的Al金属作为电极；
实施例2：退火处理单层(ZrO2)0.8(Al2O3)0.2薄膜制备过程如下：
a)将硅衬底置于丙酮中，超声清洗1分钟，去除衬底表面杂质，然后将衬底置于氢氟酸稀溶液中，去除硅衬底表面的氧化物，然后将硅衬底放置在脉冲激光沉积系统腔内的衬底台上，将多组元金属氧化物(ZrO2)0.8(Al2O3)0.2和铝(Al)靶材置于靶材底盘上，沉积腔内压强为1 ×10-5Pa；
b)利用脉冲激光沉积系统在Si衬底表面沉积一层厚度为20nm的(ZrO2)0.8(Al2O3)0.2薄膜；
c)将衬底台温度升高到850℃，沉积的(ZrO2)0.8(Al2O3)0.2薄膜在850℃下，退火处理1 小时，使(ZrO2)0.8(Al2O3)0.2薄膜中发生相分离反应，结晶温度较低的ZrO2趋向在(ZrO2)0.8(Al2O3)0.2薄膜中间部位析出，随着退火过程的进行，组分不断扩散和重新分布，晶粒逐渐粗化和长大，造成薄膜中间部位ZrO2组元较多，Al2O3组元较少，形成富ZrO2的(ZrO2)x(Al2O3)1-x，而(ZrO2)0.8(Al2O3)0.2薄膜两侧ZrO2组元较少，Al2O3组元较多，形成富Al2O3的(ZrO2)x(Al2O3)1-x，单层(ZrO2)0.8(Al2O3)0.2薄膜在退火过程中自发形成三明治电荷存储结构，其中靠近硅衬底的富Al2O3的(ZrO2)x(Al2O3)1-x层作为隧穿层，富ZrO2的(ZrO2)x(Al2O3)1-x层作为电荷存储层，远离硅衬底的富Al2O3的(ZrO2)x(Al2O3)1-x层作为阻挡层；
d)利用脉冲激光沉积系统在(ZrO2)0.8(Al2O3)0.2薄膜表面沉积一层100的Al金属作为电极。

Claims (2)

1.一种退火处理形成电荷存储结构的方法，其特征在于具体步骤如下：
a)将衬底置于丙酮中，超声清洗1分钟，去除衬底表面杂质，然后将衬底置于氢氟酸稀溶液中，去除衬底表面的氧化物，然后将衬底放置在脉冲激光沉积系统腔内的衬底台上，将多组元金属氧化物(M)x(N)1-x和铝(Al)靶材置于靶材底盘上，其中M可在ZrO2、HfO2、La2O3、TiO2中任选一种，N可在SiO2、Al2O3中任选一种，x在0.5-0.8范围内取值，脉冲激光沉积系统腔内压强为1×10-5Pa-5×10-5Pa；
b)利用脉冲激光沉积系统在衬底表面沉积一层厚度为20-30nm(M)x(N)1-x薄膜；
c)将衬底台温度升高到850℃，沉积的(M)x(N)1-x薄膜在850℃下，退火处理1小时，使(M)x(N)1-x薄膜中发生相分离反应，结晶温度较低的M趋于在(M)x(N)1-x薄膜中间部位析出，随着退火过程的进行，组分不断扩散和重新分布，晶粒逐渐粗化和长大，造成(M)x(N)1-x薄膜中间部位M组元较多，N组元较少，形成富M的(M)x(N)1-x，而(M)x(N)1-x薄膜两侧M组元较少，N组元较多，形成富N的(M)x(N)1-x，单层(M)x(N)1-x薄膜在退火过程中自发形成三明治电荷存储结构，其中靠近衬底的富N的(M)x(N)1-x层作为隧穿层，富M的(M)x(N)1-x层作为电荷存储层，远离衬底的富N的(M)x(N)1-x层作为阻挡层；
d)利用脉冲激光沉积系统在(M)x(N)1-x薄膜表面沉积一层100-200nm的Al金属作为电极。
2.如权利要求1所述的退火处理形成电荷存储结构的方法在信息存储中的应用。
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