Phonon-Assisted Diffusion in Solids from First-Principles: Unraveling a New Mechanism for Fast Diffusion

从第一原理出发的固体声子辅助扩散：揭示快速扩散的新机制

• 批准号: 1954621
• 负责人: Sara Kadkhodaei
• 金额: $ 30.7万
• 依托单位: University of Illinois at Chicago
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2020
• 资助国家: 美国
• 起止时间: 2020-08-15 至 2024-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1954621&HistoricalAwards=false
• 关键词: Phonon; Assisted; Diffusion; Solids; First

Nontechnical SummaryDiffusion of molecules in liquids and gases is familiar: perfume, for example, can diffuse in air. Diffusion also takes place in high-temperature solids, and understanding how will be key to new applications. Many technologically-relevant materials, in particular those with high operating temperatures, experience different modes of collective atomic vibrations that are highly correlated. The effect of these correlated vibrations on diffusion is poorly understood, and existing theoretical models are extremely limited in incorporating them into the diffusion description. This project addresses this limitation by (a) devising a theoretical framework that describes the mass-transport behavior affected by the correlated collective atomic vibrations, and (b) implementing a computational tool to predict the diffusion coefficient without requiring experimental input.The end product will be an open-access software toolkit with predictive capability for diffusivity, which will substantially accelerate the discovery and design of advanced materials for applications such as solid-state batteries and fuel cells. Educational activities include the development of a thorough tutorial on advanced topics in the kinetics of high-temperature materials, which will be distributed on the PI's website to provide a world-wide educational platform for students. Also, a graduate-level course about first-principles modeling for engineers will be developed by the PI.Technical SummaryThere currently exist substantial gaps in fundamental understanding and theoretical modeling of diffusion phenomena in strongly anharmonic systems. Namely, (i) the effect of anharmonic vibrations on diffusion phenomena is not well understood, and (ii) existing computational models based on the harmonic approximation of zero-temperature energy fall short of predicting diffusivity in these systems. The goal of this project is to address these gaps by introducing a theoretical framework that combines stochastic sampling techniques and ab-initio calculations to identify the diffusion pathways on an effective energy surface.The findings of this project will advance the fundamental understanding of anharmonic vibration effects on diffusion and will significantly expand the current limits of diffusion modeling capabilities. Additionally, it will provide a-priori predictive capability without requiring experimental input, which will substantially accelerate the optimization and design of new materials. The outcomes of this project will contribute to the advancement of two lines of materials research: (i) predicting diffusion properties for novel high-temperature solid phases and (ii) gaining new understanding of various diffusion-controlled processes (e.g., phase transformation, precipitate growth and coarsening, oxidation, and creep) by providing accurate diffusive mobility data for their simulation.The university is a Hispanic-serving institution, and the PI will participate in two existing programs for recruiting minority students and women to engineering at UIC. She will train undergraduates and graduate students in research, and she will give introductory lectures at local high schools and develop a new graduate-level engineering course in first-principles modeling. The PI will release open-source software as well as data on diffusivity using standard repositories.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

分子在液体和气体中的扩散是常见的：例如，香水可以在空气中扩散。 扩散也发生在高温固体中，了解如何将是新应用的关键。 许多与技术相关的材料，特别是那些具有高工作温度的材料，经历了高度相关的不同模式的集体原子振动。这些相关振动对扩散的影响知之甚少，现有的理论模型在将它们纳入扩散描述中时非常有限。本项目通过以下方式解决这一限制：（a）设计一个理论框架，描述受相关集体原子振动影响的质量输运行为;（B）实现一个计算工具，在不需要实验输入的情况下预测扩散系数。最终产品将是一个具有扩散率预测能力的开放获取软件工具包，这将大大加速用于固态电池和燃料电池等应用的先进材料的发现和设计。 教育活动包括编写关于高温材料动力学高级主题的全面教程，该教程将在PI的网站上分发，为学生提供一个全球教育平台。此外，研究生水平的课程，第一原理建模的工程师将开发的PI。技术摘要目前存在着很大的差距，在强非谐系统中的扩散现象的基本理解和理论建模。也就是说，（i）非谐振动对扩散现象的影响还没有得到很好的理解，以及（ii）现有的基于零温度能量的谐波近似的计算模型不能预测这些系统中的扩散率。该项目的目标是通过引入一个理论框架，结合随机采样技术和从头计算，以确定在一个有效的能量表面上的扩散pathways.该项目的研究结果将推进对扩散的非谐振动效应的基本理解，并将显着扩大目前的扩散模拟能力的限制，以解决这些差距。此外，它将提供先验预测能力，而无需实验输入，这将大大加快新材料的优化和设计。该项目的成果将有助于推进两条材料研究路线：（i）预测新型高温固相的扩散特性;（ii）获得对各种扩散控制过程的新理解（例如，相变，沉淀物生长和粗化，氧化和蠕变），通过提供准确的扩散流动性数据，他们的模拟。该大学是一个西班牙裔服务机构，PI将参加两个现有的计划，招募少数民族学生和妇女的工程在UIC。 她将在研究方面培训本科生和研究生，她将在当地高中做介绍性讲座，并在第一原理建模方面开发一门新的研究生工程课程。 PI将使用标准存储库发布开源软件以及扩散率数据。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Cluster Expansion of Alloy Theory: A Review of Historical Development and Modern Innovations

• DOI: 10.1007/s11837-021-04840-6
• 发表时间: 2021-09
• 期刊: JOM
• 影响因子: 2.6
• 作者: S. Kadkhodaei;Jorge A. Muñoz

Improving ab initio diffusion calculations in materials through Gaussian process regression

通过高斯过程回归改进材料中的从头算扩散计算

• DOI: 10.1103/physrevmaterials.8.013804
• 发表时间: 2024
• 期刊: Physical Review Materials
• 影响因子: 3.4
• 作者: Fattahpour, Seyyedfaridoddin;Kadkhodaei, Sara
• 通讯作者: Kadkhodaei, Sara

Understanding the role of anharmonic phonons in diffusion of bcc metals

了解非简谐声子在 bcc 金属扩散中的作用

• DOI: 10.1103/physrevmaterials.6.023803
• 发表时间: 2022
• 期刊: Physical Review Materials
• 影响因子: 3.4
• 作者: Fattahpour, Seyyedfaridoddin;Davariashtiyani, Ali;Kadkhodaei, Sara
• 通讯作者: Kadkhodaei, Sara

Phonon-assisted diffusion in bcc phase of titanium and zirconium from first principles

根据第一原理，钛和锆的 bcc 相中的声子辅助扩散

• DOI: 10.1103/physrevmaterials.4.043802
• 发表时间: 2020
• 期刊: Physical Review Materials
• 影响因子: 3.4
• 作者: Kadkhodaei, Sara;Davariashtiyani, Ali
• 通讯作者: Davariashtiyani, Ali

Predicting synthesizability of crystalline materials via deep learning

• DOI: 10.1038/s43246-021-00219-x
• 发表时间: 2021-11-18
• 期刊: COMMUNICATIONS MATERIALS
• 影响因子: 7.8
• 作者: Davariashtiyani, Ali;Kadkhodaie, Zahra;Kadkhodaei, Sara
• 通讯作者: Kadkhodaei, Sara