A Janovec-Kay-Dunn-Like Behavior at Thickness Scaling in Ultra-Thin Antiferroelectric ZrO2 Films,Advanced Electronic Materials

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A Janovec-Kay-Dunn-Like Behavior at Thickness Scaling in Ultra-Thin Antiferroelectric ZrO2 Films
Advanced Electronic Materials ( IF 5.3 ) Pub Date : 2021-09-12 , DOI: 10.1002/aelm.202100485
Nujhat Tasneem ₁ , Yasmin Mohamed Yousry ₂ , Mengkun Tian ₃ , Milan Dopita ₄ , Sebastian E. Reyes‐Lillo ₅ , Josh Kacher ₆ , Nazanin Bassiri‐Gharb _{2,

6} , Asif Islam Khan _{1,

6}

Affiliation

Originally based on phenomenological observations, the Janovec–Kay–Dunn (JKD) scaling law has been historically used to describe the dependence of the ferroelectric coercive fields (E_c) on a critical length scale of the material, wherein the film thickness (t) is considered the length scale, and E_c ∝ t^−2/3. Here, for the first time, a JKD-type scaling behavior is reported in an antiferroelectric material, using the ultra-thin films of prototypical flourite-structure binary oxide, zirconia. In these films, a decrease in the ZrO₂ layer thickness from 20 nm to 5.4 nm leads to an increase in critical fields for both nonpolar-to-polar (E_a), and polar-to-nonpolar (E_f) transitions, accompanied by a decrease in the average crystallite size, and an increase in the tetragonal distortion of the non-polar P4₂/nmc ground state structure. Notably, the -2/3 power law as in the JKD law holds when average crystallite size (d), measured from glancing-incident X-ray diffraction, is considered as the critical length scale—i.e., E_a, E_f ∝ d^−2/3. First principles calculations suggest that the increase of tetragonality in thinner films contributes to an increase of the energy barrier for the transition from the non-polar tetragonal ground state to the field-induced polar orthorhombic phase, and in turn, an increase in E_a critical fields. These results suggest a de-stabilization of the ferroelectric phase with a decreasing thickness in antiferroelectric ZrO₂, which is contrary to the observations in its fluorite-structure ferroelectric counterparts. With the recent interests in utilizing antiferroelectricity for advanced semiconductor applications, our fundamental exposition of the thickness dependence of functional responses therein can accelerate the development of miniaturized, antiferroelectric electronic memory elements for the complementary metal-oxide-semiconductor based high-volume manufacturing platforms.

中文翻译：

超薄反铁电 ZrO2 薄膜厚度缩放时的类似 Janovec-Kay-Dunn 的行为

最初基于现象观察，Janovec-凯邓恩（JKD）比例定律历来被用于描述的铁电体的矫顽场（的依赖性Ë _Ç上的材料的临界长度尺度，），其中所述膜的厚度（吨）被认为是长度尺度，并且E _c ∝ t ^−2/3。在这里，首次报道了使用原型氟石结构二元氧化物氧化锆超薄膜在反铁电材料中的 JKD 型缩放行为。在这些薄膜中，ZrO ₂层厚度从 20 nm 减少到 5.4 nm 导致非极性到极性 ( E _a)，以及极性到非极性 ( E _f ) 的转变，伴随着平均微晶尺寸的减小，以及非极性P 4 ₂ / nmc基态结构的四方畸变的增加。值得注意的是，JKD 定律中的 -2/3 幂定律适用于当从掠射入射 X 射线衍射测量的平均微晶尺寸 ( d ) 被认为是临界长度尺度i 时。e ., E _a , E _f ∝ d ^−2/3. 第一性原理计算表明，较薄薄膜中四方性的增加有助于增加从非极性四方基态到场诱导的极性正交相转变的能垒，进而增加E _a临界值领域。这些结果表明铁电相随着反铁电 ZrO ₂厚度的减小而不稳定，这与其萤石结构铁电对应物的观察结果相反。随着最近在先进半导体应用中利用反铁电性的兴趣，我们对其中功能响应的厚度依赖性的基本阐述可以加速基于互补金属氧化物半导体的大批量制造平台的小型化反铁电电子存储元件的开发。

更新日期：2021-11-10

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