(Semi)-local density functional approximations (DFAs) suffer from self-interaction error (SIE). When the first ionization energy (IE) is computed as the negative of the highest-occupied orbital (HO) eigenvalue, DFAs notoriously underestimate them compared to quasi-particle calculations. The inaccuracy for the HO is attributed to SIE inherent in DFAs. We assessed the IE based on Perdew-Zunger self-interaction corrections on 14 small to moderate-sized organic molecules relevant in organic electronics and polymer donor materials. Though self-interaction corrected DFAs were found to significantly improve the IE relative to the uncorrected DFAs, they overestimate. However, when the self-interaction correction is interiorly scaled using a function of the iso-orbital indicator zσ, only the regions where SIE is significant get a correction. We discuss these approaches and show how these methods significantly improve the description of the HO eigenvalue for the organic molecules.
Calculated state-of-the art results for solvation and ionization energies of thousands of organic molecules relevant to battery design
Ecole Polytechnique Fédérale de Lausanne（洛桑联邦理工学院）；University of Vienna（维也纳大学）；Uppsala University（乌普萨拉大学）；Vector Institute for Artificial Intelligence（人工智能向量研究所）；University of Toronto（多伦多大学）；Technische Universität Berlin（柏林工业大学）
Machine Learning for Screening Large Organic Molecules
有机半导体是廉价、可扩展和可持续的电子器件、发光二极管和光电子器件的有前途的材料。对于有机光电池来说，在广阔的化合物空间中寻找具有合适性质的化合物是一个挑战。例如，电离能应该适合太阳光的光谱，并且能级必须允许有效的电荷传输。在这里，开发了一种机器学习模型，用于快速准确地估计给定分子结构的HOMO和LUMO能量。它建立在SchNet模型（Schütt et al.（2018））的基础上，并增加了“Set 2Set”读出模块（Vinyals et al.（2016））。Set 2Set模块比求和和平均聚合具有更强的表达能力，更适合于所考虑的复杂量。大多数以前的模型都是在相当小的分子上训练和评估的。因此，第二个贡献是通过添加来自其他来源的更大分子并建立一致的训练/验证/测试分割来扩展机器学习方法的范围。作为第三个贡献，我们做了一个多任务分析，以解决来自不同理论层次的不同来源的问题。所有这三个贡献结合起来，使模型的准确性接近化学准确性。
The Astrochemistry Low-energy Electron Cross-Section (ALeCS) database I. Semi-empirical electron-impact ionization cross-section calculations and ionization rates
Ionization Energies, Electron Affinities, Bandgaps, Exciton Binding Energies, and Polarization Energies of Orientation-Controlled Picene, [6]-Phenacene, and [7]-Phenacene Thin Films
Chiba University（千叶大学）；Kyushu Institute of Technology（九州工业大学）；Institute for Molecular Science, National Institutes of Natural Sciences（国立自然科学研究所分子科学研究所）；The Graduate University for Advanced Studies (SOKENDAI)（综合研究大学院大学）
