采用量子含时波包方法研究H/D+Li2LiH/LiD+Li反应

李文涛; 于文涛; 姚明海

doi:10.7498/aps.67.20180324

留言板

尊敬的读者、作者、审稿人, 关于本刊的投稿、审稿、编辑和出版的任何问题, 您可以本页添加留言。我们将尽快给您答复。谢谢您的支持!

姓名

邮箱

手机号码

标题

留言内容

验证码

摘要

采用量子波包方法和二阶分裂算符方法对H/D+Li2LiH/LiD+Li反应在0.01到0.4 eV的碰撞能范围内进行了动力学计算.在态分辨的理论水平上计算了反应概率、积分截面、微分截面等动力学性质并与之前的理论结果进行了比较.结果表明：由于本文的计算中包含了总角动量J在体固定坐标轴上的所有投影所得，结果更加精确；此外，当H原子被重的同位素原子D取代，反应概率、积分截面增大，然而这并没有对反应机理产生大的影响.前后对称的微分截面表明插入反应机理在反应过程中占据主导地位.

关键词:

作者及机构信息

1.
渤海大学基础教研部, 锦州 121000;

2.
中国科学院大连化学物理研究所, 分子反应动力学国家重点实验室, 大连 116023;

3.
东风县第三中学, 辽源 136300

通信作者: 李文涛, wtlee1982@163.com

基金项目: 辽宁省博士科学基金（批准号：201601349）和辽宁省教育厅青年项目（批准号：LQ2017001）资助的课题.

参考文献

[1]	Chu T S, Zhang Y, Han K L 2006 Int. Rev. Phys. Chem. 25 201
[2]	Prez-Ros J, Greene C H 2015 J. Chem. Phys. 143 041105
[3]	Wang B B, Han Y C, Cong S L 2016 J. Chem. Phys. 145 204304
[4]	Wang B B, Han Y C, Gao W, Cong S L 2017 Phys. Chem. Chem. Phys. 19 22926
[5]	Wu C H, Ihle H R 1977 J. Chem. Phys. 66 4356
[6]	Kim S K, Herschbach D R 1987 Faraday Discuss. Chem. Soc. 84 159
[7]	Vezin B, Dugourd P, Rayane D, Labastie P, Broyer M 1993 Chem. Phys. Lett. 202 209
[8]	Siegbahn P, Schaefer H F 1975 J. Chem. Phys. 62 3488.
[9]	Yan G S, Xian H, Xie D Q 1997 Sci. China Ser. B:Chem. 40 342
[10]	Maniero A M, Acioli P H, Silva G M, Gargano R 2010 Chem. Phys. Lett. 490 123
[11]	Song Y Z, Li Y Q, Gao S B, Meng Q T 2014 Eur. Phys. J. D 68 3
[12]	Yuan M L, Li W T, Chen M D 2017 Int. J. Quant. Chem. e25380
[13]	Kim S K, Jeoung S C, Tan A L C, Herschbach D R 1991 J. Chem. Phys. 95 3854
[14]	Vila H V R, Leal L A, Martins J B L, Skouteris D, eSilva G M, Gargano R 2012 J. Chem. Phys. 136 34319
[15]	Cunha W F, Leal L A, Cunha T F, Silva G M, Martins J B L, Gargano R 2014 J. Mol. Model 20 2315
[16]	Gao S B, Zhang J, Song Y Z, Meng Q T 2015 Eur. Phys. J. D 69 111
[17]	Gao S B, Zhang L, Song Y Z, Meng Q T 2016 Chem. Phys. Lett. 651 233
[18]	Fu B N, Zhang D H 2012 J. Chem. Phys. 136 194301
[19]	Shen P R, Han Y C, Li J L, Chen C J, Cong S L 2015 Laser Phys. Lett. 12 045302
[20]	Pang Y H, Wang B B, Han Y C, Cong S L, Niu Y Y 2016 Chin. J. Chem. Phys. 29 297
[21]	Gao W, Wang B B, Hu X J, Chai S, Han Y C, Greenwood J B 2017 Phys. Rev. A 96 013426
[22]	Yuan J C, Cheng D H, Chen M D 2014 RSC Adv. 4 36189
[23]	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 物理学报 63 063402]
[24]	Zhang J, Wei W, Gao S B, Meng Q T 2015 Acta Phys. Sin. 64 063101 (in Chinese)[张静,魏巍,高守宝,孟庆田 2015 物理学报 64 063101]
[25]	Yuan K J, Cheng Y, Liu X H, Harich S, Yang X M, Zhang D H 2006 Phys. Rev. Lett. 96 103202
[26]	Hankel M, Smith S C, Allan R J, Gray S K, Balint-Kurti G G 2006 J. Chem. Phys. 125 164303
[27]	Fu B, Zhang D H 2007 J. Phys. Chem. A 111 9516
[28]	Zhang D H 2006 J. Chem. Phys. 125 133102
[29]	Kosloff R 1988 J. Phys. Chem. 92 2087
[30]	Light J C, Carrington T 2000 Adv. Chem. Phys. 114 263

施引文献

[1]	Chu T S, Zhang Y, Han K L 2006 Int. Rev. Phys. Chem. 25 201
[2]	Prez-Ros J, Greene C H 2015 J. Chem. Phys. 143 041105
[3]	Wang B B, Han Y C, Cong S L 2016 J. Chem. Phys. 145 204304
[4]	Wang B B, Han Y C, Gao W, Cong S L 2017 Phys. Chem. Chem. Phys. 19 22926
[5]	Wu C H, Ihle H R 1977 J. Chem. Phys. 66 4356
[6]	Kim S K, Herschbach D R 1987 Faraday Discuss. Chem. Soc. 84 159
[7]	Vezin B, Dugourd P, Rayane D, Labastie P, Broyer M 1993 Chem. Phys. Lett. 202 209
[8]	Siegbahn P, Schaefer H F 1975 J. Chem. Phys. 62 3488.
[9]	Yan G S, Xian H, Xie D Q 1997 Sci. China Ser. B:Chem. 40 342
[10]	Maniero A M, Acioli P H, Silva G M, Gargano R 2010 Chem. Phys. Lett. 490 123
[11]	Song Y Z, Li Y Q, Gao S B, Meng Q T 2014 Eur. Phys. J. D 68 3
[12]	Yuan M L, Li W T, Chen M D 2017 Int. J. Quant. Chem. e25380
[13]	Kim S K, Jeoung S C, Tan A L C, Herschbach D R 1991 J. Chem. Phys. 95 3854
[14]	Vila H V R, Leal L A, Martins J B L, Skouteris D, eSilva G M, Gargano R 2012 J. Chem. Phys. 136 34319
[15]	Cunha W F, Leal L A, Cunha T F, Silva G M, Martins J B L, Gargano R 2014 J. Mol. Model 20 2315
[16]	Gao S B, Zhang J, Song Y Z, Meng Q T 2015 Eur. Phys. J. D 69 111
[17]	Gao S B, Zhang L, Song Y Z, Meng Q T 2016 Chem. Phys. Lett. 651 233
[18]	Fu B N, Zhang D H 2012 J. Chem. Phys. 136 194301
[19]	Shen P R, Han Y C, Li J L, Chen C J, Cong S L 2015 Laser Phys. Lett. 12 045302
[20]	Pang Y H, Wang B B, Han Y C, Cong S L, Niu Y Y 2016 Chin. J. Chem. Phys. 29 297
[21]	Gao W, Wang B B, Hu X J, Chai S, Han Y C, Greenwood J B 2017 Phys. Rev. A 96 013426
[22]	Yuan J C, Cheng D H, Chen M D 2014 RSC Adv. 4 36189
[23]	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 物理学报 63 063402]
[24]	Zhang J, Wei W, Gao S B, Meng Q T 2015 Acta Phys. Sin. 64 063101 (in Chinese)[张静,魏巍,高守宝,孟庆田 2015 物理学报 64 063101]
[25]	Yuan K J, Cheng Y, Liu X H, Harich S, Yang X M, Zhang D H 2006 Phys. Rev. Lett. 96 103202
[26]	Hankel M, Smith S C, Allan R J, Gray S K, Balint-Kurti G G 2006 J. Chem. Phys. 125 164303
[27]	Fu B, Zhang D H 2007 J. Phys. Chem. A 111 9516
[28]	Zhang D H 2006 J. Chem. Phys. 125 133102
[29]	Kosloff R 1988 J. Phys. Chem. 92 2087
[30]	Light J C, Carrington T 2000 Adv. Chem. Phys. 114 263

引用本文:

Citation:

计量

文章访问数: 1109
PDF下载量: 99
被引次数: 0

采用量子含时波包方法研究H/D+Li2LiH/LiD+Li反应

1. 渤海大学基础教研部, 锦州 121000;

2. 中国科学院大连化学物理研究所, 分子反应动力学国家重点实验室, 大连 116023;

3. 东风县第三中学, 辽源 136300

通信作者: 李文涛, wtlee1982@163.com

基金项目:

辽宁省博士科学基金（批准号：201601349）和辽宁省教育厅青年项目（批准号：LQ2017001）资助的课题.

收稿日期: 2018-02-11

修回日期: 2018-03-22

刊出日期: 2019-05-20

摘要: 采用量子波包方法和二阶分裂算符方法对H/D+Li2LiH/LiD+Li反应在0.01到0.4 eV的碰撞能范围内进行了动力学计算.在态分辨的理论水平上计算了反应概率、积分截面、微分截面等动力学性质并与之前的理论结果进行了比较.结果表明：由于本文的计算中包含了总角动量J在体固定坐标轴上的所有投影所得，结果更加精确；此外，当H原子被重的同位素原子D取代，反应概率、积分截面增大，然而这并没有对反应机理产生大的影响.前后对称的微分截面表明插入反应机理在反应过程中占据主导地位.

关键词:

H/D + Li2 LiH/LiD + Li reactions studied by quantum time-dependent wave packet approach

1.
Department of College Foundation Education, Bohai University, Jinzhou 121000, China;

2.
State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China;

3.
Third Senior Middle School of Dongfeng County, Liaoyuan 136300, China

Fund Project:

Project supported by the Doctoral Science Fund of Liaoning Province, China (Grant No. 201601349) and the Youth Fund of Education Department of Liaoning Province, China (Grant No. LQ2017001).

Received Date: 11 February 2018

Accepted Date: 22 March 2018

Published Online: 20 May 2019

Abstract: The isotopic effect is a significant way to further understand the reaction mechanism without greatly changing the system. However, the isotopic effect of the H + Li2 reaction has received little attention in previous theoretical studies. Furthermore, as a deep potential well exists on the reaction path, obtaining convergent result is very time-consuming. So some approximate methods were used in previous theoretical calculations. However the Coriolis coupling effect plays an important role in the reaction, and thus whether these approximate methods are reasonable needs further testing. Based on the potential energy surface (PES) reported by Song et al., the dynamical calculations of H/D + Li2 LiH/LiD + Li reactions are carried out by time dependent quantum wave packet method with second order split operator in a collision energy range from 0 to 0.4 eV. In order to obtain the convergent results, lots of convergence tests are carried out and because the Coriolis coupling effect plays an important role in the reaction, all the number of projections of total angular momentum J are included in the present calculation. The dynamical properties such as reaction probability, integral cross section, differential cross section are calculated and compared with previous theoretical values. Large discrepancies are found between present results and the values obtained from Gao et al. especially at high collision energies. Owing to the fact that the same PES is applied to the calculation and Gao's results of total angular momentum J=0 accord well with the present values, we suppose that the parameters used in the calculation have little influence on the final results and the main discrepancies are attributed to the number of projections of total angular momentum which are cut off in Gao et al.'s calculation. In order to verify our speculation, the numbers of projections of total angular momentum which are 1, 5, 10, 15, 20, and 25, are considered in the calculation, respectively. The results indicate that the main discrepancy between present values and the results obtained from Gao et al. can be attributed to the number of projections of total angular momentum used in Gao et al.'s calculation that is not convergent, and that the present values are more accurate than previous theoretical studies for all the numbers of projections of total angular momentum which are included in the calculation. Furthermore, when the H atom is substituted by the heavy isotope D atom, the reaction probability and integral cross section become large. However, it does not generate large effect on the reaction mechanism. The forward and backward symmetry differential cross section signals indicate that the complex forming reaction mechanism dominates the reaction.

Keywords:

全文HTML

参考文献 (30)

搜索

留言板