Effect of Li Termination on the Electronic and Hydrogen Storage Properties of Linear Carbon Chains: A TAO-DFT Study

Role of Kekulé and Non-Kekulé Structures in the Radical Character of Alternant Polycyclic Aromatic Hydrocarbons: A TAO-DFT Study

We investigate the role of Kekule and non-Kekule structures in the radical character of alternant polycyclic aromatic hydrocarbons (PAHs) using thermally-assisted-occupation density functional theory (TAO-DFT), an efficient electronic structure method for the study of large ground-state systems with strong static correlation effects. Our results reveal that the studies of Kekule and non-Kekule structures qualitatively describe the radical character of alternant PAHs, which could be useful when electronic structure calculations are infeasible due to the expensive computational cost. In addition…

Role of exact exchange in thermally-assisted-occupation density functional theory: A proposal of new hybrid schemes

We propose hybrid schemes incorporating exact exchange into thermally-assisted-occupation density functional theory (TAO-DFT) [J.-D. Chai, J. Chem. Phys. 136, 154104 (2012)] for an improved description of nonlocal exchange effects. With a few simple modifications, global and range-separated hybrid functionals in Kohn-Sham density functional theory (KS-DFT) can be combined seamlessly with TAO-DFT. In comparison with global hybrid functionals in KS-DFT, the resulting global hybrid functionals in TAO-DFT yield promising performance for systems with strong static correlation effects (e.g., the dis…

Electronic Properties of Cyclacenes from TAO-DFT

Owing to the presence of strong static correlation effects, accurate prediction of the electronic properties (e.g., the singlet-triplet energy gaps, vertical ionization potentials, vertical electron affinities, fundamental gaps, symmetrized von Neumann entropy, active orbital occupation numbers, and real-space representation of active orbitals) of cyclacenes with n fused benzene rings (n = 4-100) has posed a great challenge to traditional electronic structure methods. To meet the challenge, we study these properties using our newly developed thermally-assisted-occupation density functional the…

Effect of Li Adsorption on the Electronic and Hydrogen Storage Properties of Acenes: A Dispersion-Corrected TAO-DFT Study

Due to the presence of strong static correlation effects and noncovalent interactions, accurate prediction of the electronic and hydrogen storage properties of Li-adsorbed acenes with n linearly fused benzene rings (n = 3 - 8) has been very challenging for conventional electronic structure methods. To meet the challenge, we study these properties using our recently developed thermally-assisted-occupation density functional theory (TAO-DFT) with dispersion corrections. In contrast to pure acenes, the binding energies of H2 molecules on Li-adsorbed acenes are in the ideal binding energy range (a…

有限温度热辅助占据密度泛函理论，从头计算分子动力学，以及量子力学/分子力学方法

Finite-Temperature Thermally-Assisted-Occupation Density Functional Theory, Ab Initio Molecular Dynamics, and Quantum Mechanics/Molecular Mechanics Methods

本文提出有限温度TAO-DFT方法，结合从头计算分子动力学和QM/MM，用于研究n-苯并二苯并环在有限温度下的自由基性质和红外光谱。

有限温度绝热连接约化密度矩阵泛函理论：i-DMFT和TAO-DFT的统一框架

Finite-temperature adiabatic-connection reduced density-matrix functional theory: a unified framework for i-DMFT and TAO-DFT

本文提出FT-AC-RDMFT这一统一框架，将i-DMFT与TAO-DFT关联，数值计算验证其能改善化学键断裂描述，还可修正V₂O₃的LDA体模量高估问题。