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论文类型：期刊论文

发表时间：2014-11-17

发表刊物：MOLECULAR PHYSICS

收录刊物：SCIE

卷号：112

期号：22

页面范围：2945-2953

ISSN号：0026-8976

关键字：reactive mechanism; PES; QCT; TDWP

摘要：The time-dependent quantum wave packet (TDWP) and quasiclassical trajectory calculations (QCT) are carried out for the Au(S-2) + H-2(X-1 n-ary sumation (+)(g)) -> AuH(X-1 n-ary sumation (+)(g)) + H(S-2) reaction on a global potential energy surface. The reaction probabilities at a series of J values, integral cross sections (ICSs) and differential cross sections of the title reaction are calculated by the TDWP method. For reaction probabilities, there are a mass of sharp oscillations at low collision energy, which can be attributed to resonances supported by the potential well. Due to the endothermicity of the title reaction, the total ICS shows a threshold about 1.53eV. In order to further investigate the reactive mechanism, the lifetime of complex is calculated by QCT method. At the low collision energy, most intermediate complexes are long lived, which implies that the reaction is governed by indirect reactive mechanism. With the collision energy increasing, the direct reactive mechanism occupies the dominant position. Due to the change of the reactive mechanism, the angular distribution shifts toward the forward direction with collision energy increasing. The isotopic variant, Au + D-2 -> AuD + D reaction, is also calculated by TDWP method. The calculated reaction probabilities and ICSs show that the isotope effect reduces the reactivity.