Six-dimensional quantum dynamics for dissociative chemisorption of H2 and D2 on Ag(111) on a permutation invariant potential energy surface

被引:66
作者
Jiang, Bin [1 ]
Guo, Hua [1 ]
机构
[1] Univ New Mexico, Dept Chem & Chem Biol, Albuquerque, NM 87131 USA
基金
美国国家科学基金会;
关键词
CHEMICALLY ACCURATE SIMULATION; AUGMENTED-WAVE METHOD; RECOMBINATIVE DESORPTION; NEURAL-NETWORKS; REACTIVE SCATTERING; SUBSURFACE OXYGEN; METAL-SURFACES; BASIS-SET; HYDROGEN; CU(111);
D O I
10.1039/c4cp03761h
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
A six-dimensional potential energy surface (PES) for H-2 dissociation on rigid Ag(111) is developed by fitting similar to 4000 plane-wave density functional theory points using the recently proposed permutation invariant polynomial-neural network (PIP-NN) method, which enforces both the surface periodicity and molecular permutation symmetry. Quantum reactive scattering calculations on the PIP-NN PES yielded dissociative sticking probabilities for both H-2 and D-2. Good agreement with experiment was achieved at high collision energies, but the agreement is less satisfactory at low collision energies, due apparently to the neglect of surface temperature in our model. The dissociation is activated by both vibrational and translational excitations, with roughly equal efficacies. Rotational and alignment effects were examined and found to be quite similar to hydrogen dissociation on Ag(100) and Cu(111).
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页码:24704 / 24715
页数:12
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