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利用含时量子波包动力学理论在HLi2 基态势能面上研究了H+Li2 → LiH+Li 反应的动力学性质. 计算得到了体系在0-0.4 eV 范围内J = 0 不同振动量子数(v = 0, 1, 2, 3), v = 0 不同转动量子数(J = 0, 5, 10,15) 下的反应概率、积分反应截面和热速率常数, 在此基础上讨论了释能反应的反应阈能随总角动量量子数的变化规律以及振动量子数对反应概率的影响等问题. 研究发现, 随着转动量子数的增大, 反应阈能也在逐渐增大; 然而随着振动量子数的增大, 由于反应为释能反应, 反应发生的概率却在逐渐减小. 分析了碰撞能对积分散射截面的影响以及温度对反应速率常数影响的规律.In this paper, the time-dependent wave-packet method is used to study the three-dimensional dynamical properties of the H+Li2 reactive system on its ground state potential energy surface. The reaction probabilities for J=0 with different vibrational quantum numbers v=0, 1, 2, 3 and for v=0 with different total rotational quantum numbers, integral cross sections and rate constants are calculated for collision energies in a range between 0 and 0.4 eV. The features of the reaction probabilities and reaction threshold energy are analyzed. The results show that the vibrational excitation has a certain inhibitory effect on the reaction process and the reaction threshold energy increases with the increase of J. These phenomena are associated with the type of the exothermic reaction of the reactive system. The influence of the collision energy on the integral cross sections and the effect of the temperature on reaction rate constants are also investigated.
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Keywords:
- time dependent quantum scattering theory /
- reaction probability /
- integral cross section /
- H+Li2
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[28] Meijer A J H M, Goldfield E M, Gray S K, Balint-Kurti G G 1998 Chem. Phys. Lett. 293 270
[29] Beärda R A, van Hemert M C, van Dishoeck E F 1992 J. Chem. Phys. 97 8240
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[1] Lee Y T, Gordon R J, Herschbach D R 1971 J. Chem. Phys. 54 2410
[2] Wu C H, Ihle H R 1977 J. Chem. Phys. 66 4356
[3] Vezin B, Dugourd Ph, Rayane D, Labastie P, Broyer M 1993 Chem. Phys. Lett. 202 209
[4] Antoine R, Dugourd Ph, Rayane D, Allouche A R, Aubert-Frécon M, Broyer M 1996 Chem. Phys. Lett. 261 670
[5] Shukla C P, Sathyamurthy N, Khuller I P 1987 J. Chem. Phys. 87 3251
[6] Kim S K, Jeoung S C, Tan A L C, Herschbach D R 1991 J. Chem. Phys. 95 3854
[7] Guosen Y, Hui X, Xie D 1997 Sci. China 40 342
[8] Maniero A M, Acioli P H, e Silva G M, Gargano R 2010 Chem. Phys. Lett. 490 123
[9] Vila H V R, Leal L A, Martins J B L, Skouteris D, e Silva G M, Gargano R 2012 J. Chem. Phys. 136 134319
[10] Song Y Z, Li Y Q, Gao S B, Meng Q T 2014 Eur. Phys. J. D 68 3
[11] da Cunha W F, Leal L A, da Cunha T F, e Silva G M, Gargano R, Martins J B L 2014 J. Mol. Model 20 2315
[12] Kuppermann A, Schatz G C 1975 J. Chem. Phys. 62 2502
[13] Redmon M J, Wyatt R E 1979 Chem. Phys. Lett. 63 209
[14] Hutson J M, Schwartz C 1983 J. Chem. Phys. 79 5179
[15] Schatz G C, Kuppermann A 1976 J. Chem. Phys. 65 4642
[16] Kuppermann A, Kaye J A, Dwyer J P 1980 Chem. Phys. Lett. 74 257
[17] Clary D C 1991 J. Chem. Phys. 95 7298
[18] Deng C H, Feng D C, Cai Z T 1994 Sci. China B 37 1025
[19] Schnieder L, Seekamp-Rahn K, Borkowski J, Wrede E, Welge K H, Aoiz F J, Bañiares L, D'Mello M J, Herrero V J, Rábanos V S, Wyatt R E 1995 Science 269 207
[20] Zhang D H, Zhang J Z H 1993 J. Chem. Phys. 99 5615
[21] Duan Z X, Qiu M H, Yao C X 2014 Acta Phys. Sin. 63 063402 (in Chinese) [段志欣, 邱明辉, 姚翠霞 2014 63 063402]
[22] Wang Y H, Xiao C Y, Deng K M, Lu R F 2014 Chin. Phys. B 23 043401
[23] Xie T X, Zhang Y, Zhao M Y, Han K L 2003 Phys. Chem. Chem. Phys. 5 2034
[24] Liu X G, Zhang Q G, Zhang Y C, Wang M L, Zhang Z H 2004 Chin. Phys. 13 1013
[25] Chu T S, Zhang Y, Han K L 2006 Int. Rev. Phys. Chem. 25 201
[26] Chu T S, Han K L 2008 Phys. Chem. Chem. Phys. 10 2431
[27] Tal-Ezer H, Kosloff R 1984 J. Chem. Phys. 81 3967
[28] Meijer A J H M, Goldfield E M, Gray S K, Balint-Kurti G G 1998 Chem. Phys. Lett. 293 270
[29] Beärda R A, van Hemert M C, van Dishoeck E F 1992 J. Chem. Phys. 97 8240
[30] Song Y Z, Varandas A J C 2011 J. Phys. Chem. A 115 5274
[31] Varandas A J C 1989 J. Chem. Phys. 90 4379
[32] Sun Z P, Zhang C F, Lin S Y, Zheng Y J, Meng Q T, Bian W S 2013 J. Chem. Phys. 139 014306
[33] Wei W, Gao S B, Sun Z P, Song Y Z, Meng Q T 2014 Chin. Phys. B 23 073101
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