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Br2分子在360610 nm的光解离动力学研究

秦朝朝 黄燕 彭玉峰

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Br2分子在360610 nm的光解离动力学研究

秦朝朝, 黄燕, 彭玉峰

Photodissociation dynamics of Br2 in wavelength range of 360-610 nm

Qin Chao-Chao, Huang Yan, Peng Yu-Feng
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  • 利用包含转动自由度在内的含时薛定谔方程研究了Br2分子在波长范围为360610 nm的光解离动力学.通过计算得到了Br2分子在四个特征波长处的切片解离影像,并经过分析得到了与切片解离影像相对应的动能分布;计算了Br2分子在波长范围为360610 nm内总的动能分布,以及从A,B和C三个电子态解离的碎片各自所对应的动能分布;计算了A,B和C三个电子态各自的解离概率以及碎片产物的分支比(Br*/(Br+Br*))随波长的变化.
    We study the photodissociation of Br2 in a wavelength range from 360 nm to 610 nm in the near-visible UV continuum band based on the calculation of time-dependent quantum wave packet including the rotational degree of freedom. We calculate four representative samples of two-dimensional (2D) slice images taken from photolysis of Br2 molecules, in which the different rings in the 2D slice images are corresponding to the different photodissiation channels. The radius of each 2D slice image ring is positively related to kinetic energy of photofragment. The maximum photofragment flux perpendicular or parallel to the photolysis polarization is also related to photodissiation channel. Furthermore, we calculate the total kinetic energy distribution P(E) and the P(E) distribution from the respective electronic excited states A, B and C in the wavelength range of 360-610 nm, from which we find that the wavelengths corresponding to the maximum dissociation probability from respective electronic excited states A, B and C are 510 nm, 469 nm, and 388 nm, respectively. As is well known, not only the total dissociation probability, but also the respective dissociation probability of electronic excited states is dependent on the laser wavelength. We also calculate the dissociation probabilities from electronic excited states A, B and C, respectively. We find that the dissociation probability of electronic excited state A is not significant when 480 nm and that the peak intensity of the dissociation probability to the A state is about 13.0\% of that to the C state, while that to the B state is about 43.4\%. In addition, because the electronic excited states A and C are related to the photodissociation channel Br + Br, and the electronic excited state B is corresponding to the photodissociation channel Br + Br*, the images which reveal the involvement of more than one product channel can be analyzed by the respective channel branching ratios. At the short wavelength ( 400 nm) the branching ratio (Br*/(Br+Br*)) is small, even near to zero, which reflects that electronic state C transition gives rise to many Br + Br over Br + Br*. However, within the wavelength range (=440-500 nm) Br + Br* photofragments are excess of Br + Br, so the electronic state B transition is dominant. At longer wavelength ( 530 nm) the branching ratio (Br*/(Br+Br*)) is also low, near to zero, indicating the prevalence of electronic state A transition. Ignoring the dissociation from electronic state C, the maximum dissociation probability 469 nm is consistent with branching ratio maximum 462 nm. Because the electronic excited state C is related to the photodissociation channel Br + Br, the branching ratio will be reduced. So the maximum wavelength of branching ratio is blue shifted.
      通信作者: 秦朝朝, qinch@hotmail.com
    • 基金项目: 国家自然科学基金(批准号:U1404112,11404411)、河南省科技攻关研究项目(批准号:142102310274,172102210340)和河南省教育厅重点项目(批准号:17A140021)资助的课题.
      Corresponding author: Qin Chao-Chao, qinch@hotmail.com
    • Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. U1404112, 11404411), the Advanced Technology Research Program of Henan Province, China (Grant Nos. 142102310274, 172102210340), and the Foundation for Key Program of Education Department of Henan Province, China (Grant No. 17A140021).
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    Demyanenko A V, Potter A B, Dribinski V, Reisler H 2002 J. Chem. Phys. 117 2568

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    Rakitzis T P, Kitsopoulos T N 2002 J. Chem. Phys 116 9228

    [5]

    Nugent-Glandorf L, Scheer M, Samuels D A, Mulhisen A M, Grant E R, Yang X M, Bierbaum V M, Leone S R https://doi.org/10.1103/PhysRevLett.87.193002 2001 Phys. Rev. Lett. 87 1103

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    Nugent-Glandorf L, Scheer M, Samuels D A, Bierbaum V M, Leone S R 2002 J. Chem. Phys. 117 1063

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    Liu Y Z, Chen Y Y, Zheng G G, Jin F, Knopp G 2016 Acta Phys. Sin. 65 053302 (in Chinese)[刘玉柱, 陈云云, 郑改革, 金峰, Knopp Gregor 2016 物理学报 65 053302]

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    Liu Y Z, Xiao S R, Wang J F, He Z F, Qiu X J, Knopp G 2016 Acta Phys. Sin. 65 113301 (in Chinese)[刘玉柱, 肖韶荣, 王俊锋, 何仲福, 邱学军, Knopp Gregor 2016 物理学报 65 113301]

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    Liu Y Z, Deng X L, Li S, Guan Y, Li J, Long J Y, Zhang B 2016 Acta Phys. Sin. 65 193301 (in Chinese)[刘玉柱, 邓绪兰, 李帅, 管跃, 李静, 龙金友, 张冰 2016 物理学报 65 193301]

    [19]

    Liu Y Z, Long J Y, Xu L X, Zhang X Y, Zhang B 2017 Chin. Phys. Lett. 34 033301

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    Orr-Ewing A J 2015 Ann. Rev. Phys. Chem. 66 119

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    Orlando J J, Burkholder J B 1995 J. Phys. Chem. 99 1143

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    Tellinghuisen J 2001 J. Chem. Phys. 115 10417

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    Gomes J D, Gargano R, Martins J B L, de Macedo L G M https://doi.org/10.1021/jp4114283 2014 J. Phys. Chem. A 118 5818

    [24]

    Focsa C, Li H, Bernath P F 2000 J. Mol. Spectrosc. 200 104

    [25]

    Yukiya T, Nishimiya N, Samejima Y, Yamaguchi K, Suzuki M, Boone C D, Ozier I, Le Roy R J 2013 J. Mol. Spectrosc. 283 32

    [26]

    Jung Y J, Park M S, Kim Y S, Jung K H 1999 J. Chem. Phys. 111 4005

    [27]

    Kim T K, Park M S, Lee K W, Jung K H 2001 J. Chem. Phys. 115 10745

    [28]

    Zhu R S, Tang B F, Zhang X, Zhang B 2010 J. Phys. Chem. A 114 6188

    [29]

    Han Y C, Yuan K J, Hu W H, Yan T M, Cong S L 2008 J. Chem. Phys. 128 134303

    [30]

    Numico R, Keller A, Atabek O 1995 Phys. Rev. A 52 1298

    [31]

    Jolicard G, Atabek O 1992 Phys. Rev. A 46 5845

    [32]

    Jolicard G, Billing G D 1991 Chem. Phys. 149 261

    [33]

    Marston C C, Balintkurti G G 1989 J. Chem. Phys. 91 3571

    [34]

    Willner K, Dulieu O, Masnou-Seeuwsa F 2004 J. Chem. Phys. 120 548

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    Bandrauk A D, Shen H 1993 J. Chem. Phys. 99 1185

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  • [1]

    Davies J A, LeClaire J E, Continetti R E, Hayden C C 1999 J. Chem. Phys. 111 1

    [2]

    Ashfold M N R, Baggott J E https://doi.org/10.1002/jps.2600780520 1989 Molecular Photodissociation Dynamics (Letchorth:Wiley Press) p243

    [3]

    Demyanenko A V, Potter A B, Dribinski V, Reisler H 2002 J. Chem. Phys. 117 2568

    [4]

    Rakitzis T P, Kitsopoulos T N 2002 J. Chem. Phys 116 9228

    [5]

    Nugent-Glandorf L, Scheer M, Samuels D A, Mulhisen A M, Grant E R, Yang X M, Bierbaum V M, Leone S R https://doi.org/10.1103/PhysRevLett.87.193002 2001 Phys. Rev. Lett. 87 1103

    [6]

    Nugent-Glandorf L, Scheer M, Samuels D A, Bierbaum V M, Leone S R 2002 J. Chem. Phys. 117 1063

    [7]

    Klemm A, Kimmich R, Weber M 2001 Phys. Rev. E 63 041514

    [8]

    Han S I, Pierce K L, Pines A 2006 Phys. Rev. E 74 016302

    [9]

    Rogers L J, Ashfold M N R, Matsumi Y, Kawasaki M Whitaker B J 1996 Chem. Phys. Lett. 258 159

    [10]

    Beckert M, Greaves S J, Ashfold M N R 2003 Phys. Chem. Chem. Phys. 5 308

    [11]

    Kato H, Baba M 1995 Chem. Rev. 95 2311

    [12]

    Asano Y, Yabushita S 2003 Chem. Phys. Lett. 372 348

    [13]

    Liu Y Z, Xiao S R, Zhang C Y, Zheng G G, Chen Y Y 2012 Acta Phys. Sin. 61 193301 (in Chinese)[刘玉柱, 肖韶荣, 张成义, 郑改革, 陈云云 2012 物理学报 61 193301]

    [14]

    Zhang J, Zhang S A, Yang Y, Sun S Z, Wu H, Li J, Chen Y T, Jia T Q, Wang Z G, Kong F N, Sun Z R 2014 Phys. Rev. A 90 053428

    [15]

    Kettunen J A, Sankari A, Partanen L, Urpelainen S, Kivimki A, Huttula M 2012 Phys. Rev. A 85 062703

    [16]

    Liu Y Z, Chen Y Y, Zheng G G, Jin F, Knopp G 2016 Acta Phys. Sin. 65 053302 (in Chinese)[刘玉柱, 陈云云, 郑改革, 金峰, Knopp Gregor 2016 物理学报 65 053302]

    [17]

    Liu Y Z, Xiao S R, Wang J F, He Z F, Qiu X J, Knopp G 2016 Acta Phys. Sin. 65 113301 (in Chinese)[刘玉柱, 肖韶荣, 王俊锋, 何仲福, 邱学军, Knopp Gregor 2016 物理学报 65 113301]

    [18]

    Liu Y Z, Deng X L, Li S, Guan Y, Li J, Long J Y, Zhang B 2016 Acta Phys. Sin. 65 193301 (in Chinese)[刘玉柱, 邓绪兰, 李帅, 管跃, 李静, 龙金友, 张冰 2016 物理学报 65 193301]

    [19]

    Liu Y Z, Long J Y, Xu L X, Zhang X Y, Zhang B 2017 Chin. Phys. Lett. 34 033301

    [20]

    Orr-Ewing A J 2015 Ann. Rev. Phys. Chem. 66 119

    [21]

    Orlando J J, Burkholder J B 1995 J. Phys. Chem. 99 1143

    [22]

    Tellinghuisen J 2001 J. Chem. Phys. 115 10417

    [23]

    Gomes J D, Gargano R, Martins J B L, de Macedo L G M https://doi.org/10.1021/jp4114283 2014 J. Phys. Chem. A 118 5818

    [24]

    Focsa C, Li H, Bernath P F 2000 J. Mol. Spectrosc. 200 104

    [25]

    Yukiya T, Nishimiya N, Samejima Y, Yamaguchi K, Suzuki M, Boone C D, Ozier I, Le Roy R J 2013 J. Mol. Spectrosc. 283 32

    [26]

    Jung Y J, Park M S, Kim Y S, Jung K H 1999 J. Chem. Phys. 111 4005

    [27]

    Kim T K, Park M S, Lee K W, Jung K H 2001 J. Chem. Phys. 115 10745

    [28]

    Zhu R S, Tang B F, Zhang X, Zhang B 2010 J. Phys. Chem. A 114 6188

    [29]

    Han Y C, Yuan K J, Hu W H, Yan T M, Cong S L 2008 J. Chem. Phys. 128 134303

    [30]

    Numico R, Keller A, Atabek O 1995 Phys. Rev. A 52 1298

    [31]

    Jolicard G, Atabek O 1992 Phys. Rev. A 46 5845

    [32]

    Jolicard G, Billing G D 1991 Chem. Phys. 149 261

    [33]

    Marston C C, Balintkurti G G 1989 J. Chem. Phys. 91 3571

    [34]

    Willner K, Dulieu O, Masnou-Seeuwsa F 2004 J. Chem. Phys. 120 548

    [35]

    Bandrauk A D, Shen H 1993 J. Chem. Phys. 99 1185

    [36]

    Chu T S, Zhang Y, Han K L 2010 Int. Rev. Phys. Chem. 25 201

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出版历程
  • 收稿日期:  2017-05-08
  • 修回日期:  2017-07-05
  • 刊出日期:  2017-10-05

Br2分子在360610 nm的光解离动力学研究

  • 1. 河南师范大学物理与材料科学学院, 新乡 453007;
  • 2. 光电子技术及先进制造河南省工程实验室, 新乡 453007;
  • 3. 河南师范大学电子与电气学院, 新乡 453007
  • 通信作者: 秦朝朝, qinch@hotmail.com
    基金项目: 国家自然科学基金(批准号:U1404112,11404411)、河南省科技攻关研究项目(批准号:142102310274,172102210340)和河南省教育厅重点项目(批准号:17A140021)资助的课题.

摘要: 利用包含转动自由度在内的含时薛定谔方程研究了Br2分子在波长范围为360610 nm的光解离动力学.通过计算得到了Br2分子在四个特征波长处的切片解离影像,并经过分析得到了与切片解离影像相对应的动能分布;计算了Br2分子在波长范围为360610 nm内总的动能分布,以及从A,B和C三个电子态解离的碎片各自所对应的动能分布;计算了A,B和C三个电子态各自的解离概率以及碎片产物的分支比(Br*/(Br+Br*))随波长的变化.

English Abstract

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