摘要:
用量子力学从头算的耦合族CCSD(T)方法,使用相关一致基组aug-cc-pV5Z并加3s3p2d1f1g高斯键函数计算了Ar原子与H2分子的振转相互作用和电荷分布,采用Boys和Bernardi提出的均衡法消除了基组重叠误差(BSSE).然后用Tang-Toennies势能函数拟合得到Ar-H2体系相互作用势的解析表达式.在该相互作用势下,用密耦方法计算了Ar原子入射能量为83 meV时, Ar-H2(D2, T2)碰撞体系的散射截面.计算Ar-D2体系的微分截面与实验值比较符合很好.计算结果及分析表明,在长程吸引势的散射中,色散能起主要作用；在短程排斥势的散射中,交换能起重要作用.当碰撞参数在0.27 nm至0.47 nm的范围时, Ar-H2(D2, T2)碰撞体系的径向偶极发生两次转向。
Abstract:
Based on the ab initio coupled-cluster CCSD(T) method in quantum mechanics, the charge distribution of Ar atom and its vib-rotational interaction with H2 molecule are calculated using augmented correlation consistent basis sets aug-cc-pV5Z and 3s3p2d1f1g Gaussian bonding function, and the basis set superposition error (BSSE) is eliminated using Boy and Bernardi’s full counterpoise method. Afterwards, the analytical expression of the interaction potential of the Ar-H2 system is fitted with Tang-Toennies potential function. With this interaction potential, the scattering cross section of Ar-H2(D2, T2) collision system is calculated by using close-coupling method when the incident energy of Ar atoms is 83 meV. The calculated differential cross section of Ar-D2 collision system is consistent with the experimental results. Calculated result and analysis show that the dispersion energy plays a key role in the long-range attractive potential scattering, and the exchange energy plays an important role in the short-range repulsive potential scattering. The direction of the radial dipole of the Ar-H2 (D2, T2) collision system is turned twice in the range of impact parameters from 0.27 to 0.47 nm.
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