.png){kind=icon}
返回
Training Machine-Learned Density Functionals on Band Gaps
.png){kind=icon}
OA
AI
DOI：10.1021/acs.jctc.4c00999.png)
.png){kind=icon}
原文求助.png){kind=icon}
分享.png){kind=icon}
收藏
摘要
En 中文
The systematic underestimation of band gaps is one of the most fundamental challenges in semilocal density functional theory (DFT). In addition to hindering the application of DFT to predicting electronic properties, the band gap problem is intimately related to self-interaction and delocalization errors, which make the study of charge transfer mechanisms with DFT difficult. To expand the range of available tools for addressing the band gap problem, we design an approach for machine learning density functionals based on Gaussian processes to explicitly fit single-particle energy levels. We also introduce nonlocal features of the density matrix that are expressive enough to fit these single-particle levels. Combining these developments, we train a machine-learned functional for the exact exchange energy that predicts molecular energy gaps and reaction energies of a wide range of molecules in excellent agreement with reference hybrid DFT calculations. In addition, while being trained solely on molecular data, our model predicts reasonable formation energies of polarons in solids, showcasing its transferability and robustness. We discuss how this approach can be generalized to full exchange-correlation functionals, thus paving the way to the design of state-of-the-art functionals for the prediction of electronic properties of molecules and materials.
Keyword:
GAUSSIAN-BASIS SETS
EXCHANGE-CORRELATION
NUMBER
ATOMS
PSEUDOPOTENTIALS
THERMOCHEMISTRY
SCHEMES
期刊
IF:
5.5
论文数:
1.1W
被引数:
5.4W
机构
引用论文
Gaussian basis sets for accurate calculations on molecular systems in gas and condensed phases用于精确计算气相和凝聚相分子系统的高斯基集OAAI
OAAI分享收藏More realistic band gaps from meta-generalized gradient approximations: Only in a generalized Kohn-Sham scheme.png)
PHYSICAL REVIEW B
OAAI
PHYSICAL REVIEW BIF3.7
OAAI分享收藏Density Functional Theory of Open-Shell Systems. The 3d-Series Transition-Metal Atoms and Their Cations开壳系统的密度泛函理论。3d系列过渡金属原子及其阳离子
PREAI
分享收藏分享收藏分享收藏Foreign Educators Provide Feedback for the Improvement of International Student Teaching Experiences外籍教育工作者为改进国际学生教学体验提供反馈
PREAI
分享收藏
查看更多内容