关于H₂在Cu(100)上解离吸附的多组态含时Hartree计算

Multiconfigurational time-dependent Hartree calculations for dissociative adsorption of H2 on Cu(100).

作者信息

van Harrevelt Rob, Manthe Uwe

机构信息

Theoretische Chemie, Technische Universitat Munchen, Lichtenbergstrasse 4, 85747 Garching, Germany.

出版信息

J Chem Phys. 2004 Aug 22;121(8):3829-35. doi: 10.1063/1.1775785.

DOI:10.1063/1.1775785

Abstract

The efficiency of the multiconfigurational time-dependent Hartree (MCTDH) method for calculating the initial-state selected dissociation probability of H(2)(v=0,j=0) on Cu(100) is investigated. The MCTDH method is shown to be significantly more efficient than standard wave packet methods. A large number of single-particle functions is required to converge the initial-state selected reaction probability for dissociative adsorption. Employing multidimensional coordinates in the MCTDH ansatz (mode combination) is found to be crucial for the efficiency of these MCTDH calculations. Perspectives towards the application of the MCTDH approach to study dissociative adsorption of polyatomic molecules on surfaces are discussed.

摘要

研究了多组态含时Hartree（MCTDH）方法计算H₂（v = 0，j = 0）在Cu(100)上初始态选择解离概率的效率。结果表明，MCTDH方法比标准波包方法效率显著更高。对于解离吸附的初始态选择反应概率，需要大量单粒子函数才能收敛。发现在MCTDH假设（模式组合）中采用多维坐标对于这些MCTDH计算的效率至关重要。讨论了将MCTDH方法应用于研究多原子分子在表面解离吸附的前景。

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