Machine learning frontier orbital energies of nanodiamonds
Helmholtz-Zentrum Berlin für Materialien und Energie GmbH（亥姆霍兹柏林材料与能源研究中心）；Freie Universität Berlin（柏林自由大学）；Albert-Ludwigs-Universität Freiburg（阿尔伯特-路德维希-弗莱堡大学）；Microsoft Research AI4Science（微软研究院AI4Science）；Rice University（莱斯大学）
Thorren Kirschbaum, Börries von Seggern, Joachim Dzubiella, Annika Bande, Frank Noé
Nanodiamonds have a wide range of applications including catalysis, sensing, tribology and biomedicine. To leverage nanodiamond design via machine learning, we introduce the new dataset ND5k, consisting of 5,089 diamondoid and nanodiamond structures and their frontier orbital energies. ND5k structures are optimized via tight-binding density functional theory (DFTB) and their frontier orbital energies are computed using density functional theory (DFT) with the PBE0 hybrid functional. We also compare recent machine learning models for predicting frontier orbital energies for similar structures as they have been trained on (interpolation on ND5k), and we test their abilities to extrapolate predictions to larger structures. For both the interpolation and extrapolation task, we find best performance using the equivariant graph neural network PaiNN. The second best results are achieved with a message passing neural network using a tailored set of atomic descriptors proposed here.
Binding Energies for Successive Addition Reaction of .OH with C60 : A Laboratory for Testing Frontier Molecular Orbital Theory
研究了富勒烯C60上OH的连续加成反应。我们确认，最低能量的异构体的C60（OH）n形成一个带的羟基基团的赤道周围的C60，但问的问题是什么支配的相对稳定性的取代在不同的碳？基于Mulliken布居分析，从概念密度泛函理论、前线分子轨道理论、电荷和自旋密度等方面分析了影响区域选择性的因素。我们证实.OH是一个亲电自由基，它与C_（60）的连续反应受电荷和轨道控制。这被认为是特别的情况下，除了奇数C60（OH）2 m +1富勒烯醇，但也看到从福井函数和对偶描述符分析偶数C60（OH）2 m富勒烯醇。特别感兴趣的是凝聚自由基Fukui函数f0提供关于甚至C60（OH）2 m富勒烯醇与OH的反应性的信息的能力，当自旋密度为零时，并且观察到对偶描述符的符号的解释取决于是否对偶数C60（OH）2 m富勒烯醇或自旋-对奇数C60（OH）2 m +1富勒烯醇进行无限制计算。
Density-Functional Theory (DFT) and Time-Dependent DFT Study of the Chemical and Physical Origins of Key Photoproperties of End-Group Derivatives of the Nonfullerene Bulk Heterojunction Organic Solar Cell Acceptor Molecule IDIC
Partial Density of States Ligand Field Theory (PDOS-LFT): Recovering a LFT-Like Picture and Application to Photoproperties of Ruthenium(II) Polypyridine Complexes
