Structural Evolution and Metal–Insulator–Metal Transitions in Hafnium Oxides: Implication for Memristive Devices

IF 3.3 3区 化学 Q2 CHEMISTRY, PHYSICAL
Jinghong Zhao, Bole Chen, Ying Chang, Chunbao feng, Zhen Qin, Shichang Li, Dengfeng Li
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Abstract

Hafnium oxides have been widely studied for their application in resistive random-access memory, which is a prominent emerging technology for next-generation nonvolatile memory systems. We performed a comprehensive investigation into the stoichiometry-dependent structural evolution and the remarkable electronic properties of HfOx at ambient pressure. This study employed calculations based on density functional theory augmented by particle-swarm optimization and the ab initio random structure searching methodology. Through this approach, we identified novel phases of HfO, Hf2O3, HfO2, and Hf2O5, all of which were determined to be thermodynamically, dynamically, and mechanically stable. Analysis of the electronic structures, charge density variations, and charge transfer revealed that all identified phases primarily exhibit ionic bonding characteristics. Additionally, an examination of the lattice vibrational spectra offers detailed insights into the lattice dynamics and thermodynamic properties of the P21/c-HfO2. In particular, our theoretical predictions indicate that HfOx undergoes metal–insulator–metal transitions with increasing oxygen content, a characteristic that could be integral to its potential use as a fundamental component in resistive random-access memory devices.

Abstract Image

铪氧化物的结构演变和金属-绝缘体-金属跃迁:对忆阻器件的启示
作为下一代非易失性存储系统的重要新兴技术,氧化铪在电阻式随机存取存储器中的应用已经得到了广泛的研究。我们对HfOx在环境压力下的化学计量学依赖的结构演变和显著的电子特性进行了全面的研究。本研究采用密度泛函理论,结合粒子群优化和从头算随机结构搜索方法进行计算。通过这种方法,我们发现了HfO、Hf2O3、HfO2和Hf2O5的新相,它们都是热力学、动力学和机械稳定的。电子结构、电荷密度变化和电荷转移分析表明,所有确定的相主要表现出离子键特征。此外,对晶格振动谱的研究为P21/c-HfO2的晶格动力学和热力学性质提供了详细的见解。特别是,我们的理论预测表明,随着氧含量的增加,HfOx经历了金属-绝缘体-金属的转变,这一特性可能是其作为电阻随机存取存储设备基本组件的潜在用途所不可或缺的。
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来源期刊
The Journal of Physical Chemistry C
The Journal of Physical Chemistry C 化学-材料科学:综合
CiteScore
6.50
自引率
8.10%
发文量
2047
审稿时长
1.8 months
期刊介绍: The Journal of Physical Chemistry A/B/C is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.
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