A basis set of generalized nonspherical Gaussian functions (GGTOs) is presented and discussed. As a first example we report on Born-Oppenheimer energies of the hydrogen molecule. Although accurate results have been obtained, we conclude that H_2 is too 'simple' to allow for a substantial gain by using nonspherical functions. We rather expect that these functions may be particularly useful in calculations on large systems. A single basis set of GGTOs was used to simultaneously calculate the potential energy curves of several states within each subspace of {1,3}Σ_{g,u} symmetry. We hereby considerd the entire region of internuclear distances 0.8 < R < 1000 a.u. In particular the results for the fourth up to sixth electronic states show a high accuracy compared to calculations which invoke explicitely correlated functions, e.g. the relative accuracy is at least of the order of magnitude of 10^{-5}a.u. Energies for the 4 ^1Σ_u^+ and 4-6 ^3Σ_u^+ were improved and accurate data for the 6 ^3Σ_g^+, 5 ^1Σ_u^+, and 6 ^1Σ_u^+ state are, to the best of the authors knowledge, presented for the first time. Energy data for the seventh up to the nineth electronic state within each subspace were obtained with an estimated error of the order of magnitude of 10^{-4}a.u. The 7 ^1Σ_g^+ and the 6 ^1Σ_u^+ state were found to exhibit a very broad deep outer well at large internuclear distances.
Interactions of Hydrogen Molecules with Halogen-Containing Diatomics from Ab Initio Calculations: Spherical-Harmonics Representation and Characterization of the Intermolecular Potentials
The Hydration Structure of Carbon Monoxide by Ab Initio Methods
一氧化碳（CO）在液态水中的溶剂化作用对于理解其毒理学效应和生物化学作用具有重要意义。本文采用从头算分子动力学（AIMD）和CCSD（T）-F12计算方法，对Straub和Karplus分子力学（MM）模型计算CO（aq）的准确性进行了评估。CCSD（T）-F_（12）CO-H_2 O势能面表明，最稳定的结构对应于与C中心提供氢键的水。MM计算的表面错误地预测O原子是比C原子更强的氢键受体。AIMD模拟表明，CO像疏水溶质一样被溶剂化，与水的氢键非常有限。MM模型倾向于高估氢键的程度和高估C原子的原子半径。水化吉布斯自由能的计算值与实验值（9.3 kJ/mol calc. vs 10.7 kJ/mol实验）。CO（aq）在TIP 3 P模型水中的计算扩散系数为5.19 × 10-5 cm 2/s（计算值），是实验值2.32 x 10-5 cm 2/s的两倍以上
Ab initio Screening of a Sulfur Desorbed MoS$_2$ Photocatalyst for Nitrogen Fixation
本研究探讨无机硫脱附光触媒二硫化钼表面固氮过程中的热力学反应障碍。设计空间的研究使用密度泛函理论（DFT）的方法内的MMoS $_2$ M=Mo，Fe，Co的空间约束。讨论的重点是沿关联和解离途径的Heyrovsky型反应。对无机物的作用以及氮和氢亲和力之间的平衡的关键见解，为最大限度地减少所需过电位的最佳材料提供证据。据发现，具有较高浓度的Mo的相面对涉及氮的高反应势垒，其中具有较高浓度的Fe和Co的相面对涉及氢物种的高反应势垒。在没有动力学考虑的情况下，预测最佳相是具有Mo $_{0.75}$ Fe $_{0.25}$ S $_{2}$组成的1T相。该相被证明具有氢和氮亲和力的平衡，并且遵循解离途径，其可以通过非热方法来演化。
Formation and properties of astrophysical carbonaceous dust. I: ab-initio calculations of the configuration and binding energies of small carbon clusters
