NSF/DMR-BSF: Density Functionals for Predictive Excited-State Calculations of Solids (NSF-BSF Application)

NSF/DMR-BSF：用于预测固体激发态计算的密度泛函（NSF-BSF 应用）

基本信息

批准号：
2015991
负责人：
Jeffrey Neaton
金额：
$ 33.43万
依托单位：
University of California-Berkeley
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2020
资助国家：
美国
起止时间：
2020-12-01 至 2023-11-30
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=2015991&HistoricalAwards=false
关键词：
NSF DMR BSF Density Functionals

项目摘要

NONTECHNICAL SUMMARYThis award supports theoretical and computational research, and education to advance computational methods for predicting the properties of materials from fundamental scientific principles. The discovery and development of new materials for optoelectronic applications is significantly limited by a detailed understanding of how materials harvest light, transduce energy, and transport charge - all phenomena involving electronic excited states where the configuration of electrons leads to a higher energy than the lowest or ground state energy of the material. Existing computational methods are predictive for such processes, but they come at significant computational cost, and alternative approaches with similar accuracy would enable predictions for increasingly complex materials and for adapting such methods for materials discovery and design. This research project lays important groundwork toward the development of more efficient predictive theoretical frameworks that are complimentary to more computationally costly existing methods for electronic excited states in real materials. Central to this effort is mentoring of next-generation computational materials theorists at all age levels, with focus on active recruitment and promotion of women and other underrepresented-minority undergraduate and graduate students; and outreach through tours of local research facilities for undergraduate, elementary, and middle-school students – as well as educators – in the Bay area and beyond.TECHNICAL SUMMARYThis award supports theoretical and computational research, and education to advance computational methods for predicting the properties of materials. The electronic band structure is a fundamental property of crystalline matter. It serves as the basis for understanding charge transport properties of bulk materials. Moreover, it is a prerequisite for understanding optical properties of materials and for rationalizing the results of spectroscopic measurements. In materials and condensed matter physics, the formalism of choice for quantitative determination of the band structure has long been many-body perturbation theory (MBPT). This formalism has yielded excellent electronic structure predictions for many different classes of metals, semiconductors, and insulators. However, these predictions come at significant computational cost, and the ability to extract band structures from density functional theory (DFT), based on the single-electron energies and orbitals obtained from the solution of the Kohn-Sham equation, could alleviate this cost. This project involves a binational theoretical and computational collaboration to develop a robust framework for the first principles computational prediction of the quasiparticle band gaps, band structures, and optical spectra of complex solid-state materials with greater accuracy and efficiency than existing methodologies, by combining optimally-tuned range separated hybrid (OTRSH) density functionals with many-body perturbation theory. The PIs’ work has shown that OTRSH functionals lead to band structures and optical spectra for a broad class of molecular crystals and a set of group IV and III–V semiconductors and insulators, with the accuracy of leading-edge ab initio GW and GW-BSE approaches. Here, the PIs build on this success by advancing two important fronts simultaneously. First, the PIs will evaluate OTRSH as an effective starting point for GW and GW-BSE calculations for solids. Second, building on prior work, the PIs will explore routes to determine accurate DFT-OTRSH band structure and TDDFT-OTRSH optical properties without GW calculations. Once validated, the PIs will use OTRSH starting points to calculate the quasiparticle gap and band structure, as well as the linear absorption spectra, of an array of complex materials, including halide perovskites, important optoelectronic materials for which standard GW and GW-BSE methods have been demonstrated to be inadequate or inconsistent.The progress made thus far with OTRSH for band structure and optical spectra of solids is encouraging, as it suggests that it is in general possible to fix one parameter to the orientationally-averaged dielectric constant and then tune a single parameter – the range-separation parameter – to yield band structures and optical spectra in agreement with GW-BSE, partially or fully mitigating computational costs associated with MBPT. Given the quality of the OTRSH band structure with a single parameter, could OTRSH be an optimal starting point for GW and GW-BSE calculations of complex structurally and chemically heterogeneous systems? Additionally, it remains to be seen whether one can set this single parameter independent of GW-BSE calculations and experiment. Can it be predicted from materials properties in a computationally tractable manner, for isotropic and anisotropic materials alike? The aim of this project is to address these questions, and ultimately develop efficient approaches for understanding existing and predicting new excited-state phenomena in complex materials.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.

非技术摘要该奖项支持理论和计算研究以及教育，以推进从基本科学原理预测材料特性的计算方法。光电应用新材料的发现和开发受到对材料如何收集光、转换的详细了解的极大限制。能量和传输电荷 - 所有涉及电子激发态的现象，其中电子的配置导致比材料的最低或基态能量更高的能量，现有的计算方法可以预测此类过程，但它们的计算成本很高，具有类似精度的替代方法将能够预测日益复杂的材料，并适应这些方法进行材料发现和设计，该研究项目为开发更有效的预测理论框架奠定了重要的基础，该框架与计算成本更高的现有电子方法相辅相成。这项工作的核心是指导各个年龄段的下一代计算材料理论家，重点是积极招募和晋升女性和其他代表性不足的少数族裔本科生和研究生，并通过参观当地研究进行推广；设施湾区及其他地区的本科生、小学生和中学生以及教育工作者。技术摘要该奖项支持理论和计算研究以及教育，以推进预测材料特性的计算方法。它是理解块状材料的电荷传输特性的基础，也是理解材料光学特性和合理化材料和凝聚态物理中光谱测量结果的先决条件。长期以来，定量确定能带结构的选择是多体微扰理论（MBPT），这种形式为许多不同类别的金属、半导体和绝缘体提供了出色的电子结构预测，但这些预测的计算成本很高。，以及基于从 Kohn-Sham 方程解中获得的单电子能量和轨道，从密度泛函理论 (DFT) 中提取能带结构的能力，可以减轻这一成本。该项目涉及两国理论和计算合作。通过结合优化调整的距离分离混合（OTRSH）密度，开发一个强大的框架，用于复杂固态材料的准粒子带隙、能带结构和光谱的第一原理计算预测，其精度和效率比现有方法更高PI 的工作表明，OTRSH 泛函可得出多种分子晶体以及一组 IV 族和 III-V 族半导体和绝缘体的能带结构和光谱，凭借领先的从头算 GW 和 GW-BSE 方法的准确性，PI 在此成功的基础上同时推进两个重要领域：首先，PI 将评估 OTRSH 作为 GW 和 GW-BSE 计算的有效起点。其次，在先前工作的基础上，PI 将探索确定准确的 DFT-OTRSH 能带结构和 TDDFT-OTRSH 光学特性的途径，而无需进行 GW 计算。 PI 将使用 OTRSH 起点来计算一系列复杂材料的准粒子能隙和能带结构以及线性吸收光谱，包括卤化物钙钛矿，这是重要的光电材料，标准 GW 和 GW-BSE 方法已被证明可以不充分或不一致。迄今为止，OTRSH 在固体能带结构和光谱方面取得的进展令人鼓舞，因为它表明通常可以将一个参数固定为定向平均介电常数常数，然后调整单个参数（距离分离参数）以产生与 GW-BSE 一致的能带结构和光谱，在考虑到具有单个参数的 OTRSH 能带结构的质量的情况下，部分或完全减轻与 MBPT 相关的计算成本。，OTRSH 能否成为复杂结构和化学异质系统的 GW 和 GW-BSE 计算的最佳起点？此外，是否可以独立于 GW-BSE 计算和设置这一单一参数还有待观察。对于各向同性和各向异性材料，能否以可计算的方式从材料特性进行预测？该项目的目的是解决这些问题，并最终开发出有效的方法来理解复杂的现有激发态现象并预测新的激发态现象。该奖项反映了 NSF 的法定使命，并通过使用基金会的智力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

期刊论文数量（4）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Optimally tuned starting point for single-shot GW calculations of solids

固体单次引力波计算的最佳调整起点

DOI：
10.1103/physrevmaterials.6.053802
发表时间：
2022-05
期刊：
Physical Review Materials
影响因子：
3.4
作者：
Gant, Stephen E.;Haber, Jonah B.;Filip, Marina R.;Sagredo, Francisca;Wing, Dahvyd;Ohad, Guy;Kronik, Leeor;Neaton, Jeffrey B.
通讯作者：
Neaton, Jeffrey B.

Band gaps of crystalline solids from Wannier-localization–based optimal tuning of a screened range-separated hybrid functional

基于 Wannier 定位的筛选范围分离混合泛函的晶体固体带隙

DOI：
10.1073/pnas.2104556118
发表时间：
2021-08
期刊：
Proceedings of the National Academy of Sciences
影响因子：
0
作者：
Wing, Dahvyd;Ohad, Guy;Haber, Jonah B.;Filip, Marina R.;Gant, Stephen E.;Neaton, Jeffrey B.;Kronik, Leeor
通讯作者：
Kronik, Leeor

Band gaps of halide perovskites from a Wannier-localized optimally tuned screened range-separated hybrid functional

来自 Wannier 局域优化调谐筛选范围分离杂化函数的卤化物钙钛矿的带隙

DOI：
10.1103/physrevmaterials.6.104606
发表时间：
2022-10-13
期刊：
Physical Review Materials
影响因子：
3.4
作者：
Guy Ohad;Dahvyd Wing;Stephen E. Gant;A. Cohen;J. Haber;Francisca Sagredo;Marina R. Filip;J. Neaton;L. Kronik
通讯作者：
L. Kronik

Time‐Dependent Density Functional Theory of Narrow Band Gap Semiconductors Using a Screened Range‐Separated Hybrid Functional

使用屏蔽范围的窄带隙半导体的时间相关密度泛函理论 - 分离混合泛函