N2O+经由B2Пi←X2П跃迁的光解离机理研究

引用本文: 吴丹, 张立敏, 周丹娜. N₂O⁺经由B²П_i←X²П跃迁的光解离机理研究[J]. 物理化学学报, 2014, 30(8): 1575-1580. doi: 10.3866/PKU.WHXB201405202 shu

Citation: WU Dan, ZHANG Li-Min, ZHOU Dan-Na. Study on the Photodissociation Mechanism of N₂O⁺ via B²П_i←X²П Transitions[J]. Acta Physico-Chimica Sinica, 2014, 30(8): 1575-1580. doi: 10.3866/PKU.WHXB201405202 shu

N₂O⁺经由B²П_i←X²П跃迁的光解离机理研究

基金项目:
国家自然科学基金（21073177）资助项目

摘要:

在超声分子束条件下，利用360.50 nm的电离激光使N₂O分子经由[3+1]共振增强多光子电离（REMPI）产生纯净的N₂O⁺（X²Π（000））分子离子，用另一束解离激光在230-275 nm范围扫描获得N₂O⁺经由B²П_i←X²Π跃迁产生的光解碎片（NO⁺和N₂⁺）激发（PHOFEX）谱. 获得的光解碎片激发谱可以归属为B²П_i（00n）←X²Π（000）序列跃迁. 我们分别将线性三原子分子离子N₂O⁺中N―N伸缩振动简化成NO和N之间的简谐振动，N―O伸缩振动简化成N₂和O之间的简谐振动，用谐振子的简谐势能曲线和波函数对N₂O⁺分子离子X²Π和B²П_i电子态振动能级间跃迁的Franck-Condon因子进行计算，和实验得到的碎片离子增强谱实验强度进行比较，对前人给出的分子数据（分子平衡核间距）进行验证，讨论了N₂O⁺经由B²П_i（00n）←X²Π（000）电子态跃迁的光解离机理和碎片离子的分支比.

关键词:

English

Study on the Photodissociation Mechanism of N₂O⁺ via B²П_i←X²П Transitions

1.
Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, P. R. China
Received Date: 15 April 2014
Available Online: 18 July 2014
Fund Project:
国家自然科学基金（21073177）资助项目

Abstract:

Photofragment (NO⁺ and N₂⁺) excitation (PHOFEX) spectra of N₂O⁺ via B²П_i←X²Π transitions was obtained over the wavelength range from 230 to 275 nm by preparing N₂O⁺(X²Π(000)) ions via [3+1] resonance enhanced multiphoton ionization of N₂O molecules at 360.50 nm. On the basis of the approximation of harmonic oscillation between N and NO or between N₂ and O, the Franck-Condon factors for the B²П_i(00n)←X²Π(000) transitions of N₂O⁺ ions were calculated using the potential curves and wavefunctions of the harmonic oscillator. The results of such calculations were compared with the photodissociation spectra of the B²П_i(00n)←X²Π(000) transition so as to estimate the validity of the rotational constants and the bond length of the B²П_i state obtained from previous studies. The photodissociation mechanism of the B²П_i(00n)←X²Π(000) transitions of N₂O⁺ ions and the product branching ratios were also discussed.

Key words:

1. [1]
  
  (1) Wayne, R. P. Chemistry of Atmospheres; Clarendon: Oxford, 1991.
  (1) Wayne, R. P. Chemistry of Atmospheres; Clarendon: Oxford, 1991.
2. [2]
  (2) Climate Change 1994; Radiative Forcing of Climate Change and an Evaluation of the IPCC IS92 Emission Scenarios ; Houghton, J. T., Filho, L. G. M., Harris, N. B. Eds; Cambridge University Press: Cambridge, 1995.(2) Climate Change 1994; Radiative Forcing of Climate Change and an Evaluation of the IPCC IS92 Emission Scenarios ; Houghton, J. T., Filho, L. G. M., Harris, N. B. Eds; Cambridge University Press: Cambridge, 1995.
3. [3]
  (3) Zhen, C.; Hu, Y. H.; Liu, S. L.; Zhou, X. G. Chin. J. Chem. Phys. 2010, 26, 94. [甄承, 胡亚华, 刘世林, 周晓国. 化学物理学报, 2010, 26, 94.](3) Zhen, C.; Hu, Y. H.; Liu, S. L.; Zhou, X. G. Chin. J. Chem. Phys. 2010, 26, 94. [甄承, 胡亚华, 刘世林, 周晓国. 化学物理学报, 2010, 26, 94.]
4. [4]
  (4) Cossart-Ma s, C. J. Chem. Phys. 2001, 114, 7368. doi: 10.1063/1.1363671(4) Cossart-Ma s, C. J. Chem. Phys. 2001, 114, 7368. doi: 10.1063/1.1363671
5. [5]
  (5) Danis, P. O.;Wyttenbach, T.; Maier, J. P. J. Chem. Phys. 1988, 88, 3451. doi: 10.1063/1.453893(5) Danis, P. O.;Wyttenbach, T.; Maier, J. P. J. Chem. Phys. 1988, 88, 3451. doi: 10.1063/1.453893
6. [6]
  (6) Szarka, M. G.;Wallace, S. C. J. Chem. Phys. 1991, 95, 2336. doi: 10.1063/1.460940(6) Szarka, M. G.;Wallace, S. C. J. Chem. Phys. 1991, 95, 2336. doi: 10.1063/1.460940
7. [7]
  (7) Scheper, C. R.; Kuijt, J.; Buma,W. J.; DeLange, C. A. J. Chem. Phys. 1998, 109, 7844. doi: 10.1063/1.477431(7) Scheper, C. R.; Kuijt, J.; Buma,W. J.; DeLange, C. A. J. Chem. Phys. 1998, 109, 7844. doi: 10.1063/1.477431
8. [8]
  (8) Patsilinakou, E.;Wiedmann, R. T.; Fotakis, C.; Grant, E. R. J. Chem. Phys. 1989, 91, 3916. doi: 10.1063/1.456823(8) Patsilinakou, E.;Wiedmann, R. T.; Fotakis, C.; Grant, E. R. J. Chem. Phys. 1989, 91, 3916. doi: 10.1063/1.456823
9. [9]
  (9) Dehmer, P. M.; Dehmer, J. L. J. Chem. Phys. 1980, 73, 126. doi: 10.1063/1.439906(9) Dehmer, P. M.; Dehmer, J. L. J. Chem. Phys. 1980, 73, 126. doi: 10.1063/1.439906
10. [10]
  (10) Cvitas, T.; Klasinc, L.; Kovac, B. J. Chem. Phys. 1983, 79, 1567.(10) Cvitas, T.; Klasinc, L.; Kovac, B. J. Chem. Phys. 1983, 79, 1567.
11. [11]
  (11) Orth, R. G.; Dunbar, R. C. J. Chem. Phys. 1977, 66, 1619.(11) Orth, R. G.; Dunbar, R. C. J. Chem. Phys. 1977, 66, 1619.
12. [12]
  (12) Alagia, M.; Candori, P.; Falcinelli, S.; Lavollée, M.; Pirani, F.; Richter, R.; Strangers, S., Vecchiocattivi, F. Chemical Physics Letters 2006, 432, 398. doi: 10.1016/j.cplett.2006.10.100(12) Alagia, M.; Candori, P.; Falcinelli, S.; Lavollée, M.; Pirani, F.; Richter, R.; Strangers, S., Vecchiocattivi, F. Chemical Physics Letters 2006, 432, 398. doi: 10.1016/j.cplett.2006.10.100
13. [13]
  (13) Nenner, I.; Guyon, P.; Baer, T.; vers, T. R. J. Chem. Phys. 1980, 72, 6587. doi: 10.1063/1.439115(13) Nenner, I.; Guyon, P.; Baer, T.; vers, T. R. J. Chem. Phys. 1980, 72, 6587. doi: 10.1063/1.439115
14. [14]
  (14) Chen,W.; Liu, J. J. Phys. Chem. A 2003, 107, 8086. doi: 10.1021/jp022389d(14) Chen,W.; Liu, J. J. Phys. Chem. A 2003, 107, 8086. doi: 10.1021/jp022389d
15. [15]
  (15) Koppel, H.; Cederbaum, L. S.; Domcke,W. Chemical Physics1982, 69, 175. doi: 10.1016/0301-0104(82)88144-5(15) Koppel, H.; Cederbaum, L. S.; Domcke,W. Chemical Physics1982, 69, 175. doi: 10.1016/0301-0104(82)88144-5
16. [16]
  (16) Danis, P. O.;Wyttenbach, T.; Maier, J. P. J. Chem. Phys. 1988, 88, 3453.(16) Danis, P. O.;Wyttenbach, T.; Maier, J. P. J. Chem. Phys. 1988, 88, 3453.
17. [17]
  (17) Zhang, L. M.; Chen, J.; Xu, H. F.; Dai, J. H.; Liu, S. L.; Ma, X. X. J. Chem. Phys. 2001, 114, 1078.(17) Zhang, L. M.; Chen, J.; Xu, H. F.; Dai, J. H.; Liu, S. L.; Ma, X. X. J. Chem. Phys. 2001, 114, 1078.
18. [18]
  (18) Zhang, L. M.;Wang, F.;Wang, Z.; Yu, S. Q.; Liu, S. L.; Ma, X. X. J. Phys. Chem. A 2004, 108, 1342. doi: 10.1021/jp036820q(18) Zhang, L. M.;Wang, F.;Wang, Z.; Yu, S. Q.; Liu, S. L.; Ma, X. X. J. Phys. Chem. A 2004, 108, 1342. doi: 10.1021/jp036820q
19. [19]
  (19) Zhuang, X. J.; Zhang, L. M.;Wang, J. T.; Ma, Y. C.;Wang, Z.; Yu, S. Q. Chin. J. Chem. Phys. 2005, 18, 657.(19) Zhuang, X. J.; Zhang, L. M.;Wang, J. T.; Ma, Y. C.;Wang, Z.; Yu, S. Q. Chin. J. Chem. Phys. 2005, 18, 657.
20. [20]
  (20) Zhuang, X. J.; Zhang, L. M.;Wang, J. T.; Ma, Y. C.; Yu, S. Q.; Liu, S. L.; Ma, X. X. J. Phys. Chem. A 2006, 110, 6256.(20) Zhuang, X. J.; Zhang, L. M.;Wang, J. T.; Ma, Y. C.; Yu, S. Q.; Liu, S. L.; Ma, X. X. J. Phys. Chem. A 2006, 110, 6256.
21. [21]
  (21) Zhou, D. N.; Zhang, L. M.; Chen, L.;Wu, D. Acta Phys. -Chim. Sin. 2012, 28, 963. [周丹娜, 张立敏, 陈琳, 吴丹. 物理化学学报, 2012, 28, 963.] doi: 10.3866/PKU.WHXB201202162(21) Zhou, D. N.; Zhang, L. M.; Chen, L.;Wu, D. Acta Phys. -Chim. Sin. 2012, 28, 963. [周丹娜, 张立敏, 陈琳, 吴丹. 物理化学学报, 2012, 28, 963.] doi: 10.3866/PKU.WHXB201202162
22. [22]
  (22) Zhou, D. N.; Zhang, L. M.; Chen, L.;Wu, D. Chin. J. Chem. Phys. 2013, 26, 265. [周丹娜, 张立敏, 陈琳, 吴丹. 化学物理学报, 2013, 26, 265.] doi: 10.1063/1674-0068/26/03/265-269(22) Zhou, D. N.; Zhang, L. M.; Chen, L.;Wu, D. Chin. J. Chem. Phys. 2013, 26, 265. [周丹娜, 张立敏, 陈琳, 吴丹. 化学物理学报, 2013, 26, 265.] doi: 10.1063/1674-0068/26/03/265-269
23. [23]
  (23) Ma, Y. C.; Zhang, L. M.; Zhuang, X. J.;Wang, J. T.; Yang, M. P.; Yu, S. Q. Acta Phys. -Chim. Sin. 2006, 22, 1532. [马玉超, 张立敏, 庄秀娟, 王金婷, 杨茂萍, 俞书勤. 物理化学学报, 2006, 22, 1532.] doi: 10.1016/S1872-1508(06)60078-8(23) Ma, Y. C.; Zhang, L. M.; Zhuang, X. J.;Wang, J. T.; Yang, M. P.; Yu, S. Q. Acta Phys. -Chim. Sin. 2006, 22, 1532. [马玉超, 张立敏, 庄秀娟, 王金婷, 杨茂萍, 俞书勤. 物理化学学报, 2006, 22, 1532.] doi: 10.1016/S1872-1508(06)60078-8
24. [24]
  (24) Jolma, K.; Kauppinen, J.; Horneman, V. M. J. Mol. Spectrosc. 1983, 101, 278. doi: 10.1016/0022-2852(83)90133-9(24) Jolma, K.; Kauppinen, J.; Horneman, V. M. J. Mol. Spectrosc. 1983, 101, 278. doi: 10.1016/0022-2852(83)90133-9
25. [25]
  (25) Toth, R. A. Appl. Opt. 1991, 30, 5289. doi: 10.1364/AO.30.005289(25) Toth, R. A. Appl. Opt. 1991, 30, 5289. doi: 10.1364/AO.30.005289
26. [26]
  (26) Chambaud, G.; Gritli, H.; Rosmus, P.;Werner, H. J.; Knowles, P. J. Molecular Physics 2000, 98, 1793.
  (26) Chambaud, G.; Gritli, H.; Rosmus, P.;Werner, H. J.; Knowles, P. J. Molecular Physics 2000, 98, 1793.

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

N₂O⁺经由B²П_i←X²П跃迁的光解离机理研究

English

Study on the Photodissociation Mechanism of N₂O⁺ via B²П_i←X²П Transitions

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