飞秒时间分辨的光电子影像对3-甲基吡啶分子超快动力学研究

引用本文: 布玛丽亚·阿布力米提, 朱荣淑, 邱学军, 秦晨, 张冰. 飞秒时间分辨的光电子影像对3-甲基吡啶分子超快动力学研究[J]. 物理化学学报, 2014, 30(1): 22-27. doi: 10.3866/PKU.WHXB201311122 shu

Citation: ABULIMITI Bumaliya, ZHU Rong-Shu, QIU Xue-Jun, QIN Chen, ZHANG Bing. Studies of Ultrafast Dynamics of 3-Picoline with Femtosecond Time-Resolved Photoelectron Imaging[J]. Acta Physico-Chimica Sinica, 2014, 30(1): 22-27. doi: 10.3866/PKU.WHXB201311122 shu

飞秒时间分辨的光电子影像对3-甲基吡啶分子超快动力学研究

基金项目:
国家自然科学基金(91121006，21273274)资助项目 (91121006，21273274)

摘要:

利用飞秒时间分辨的光电子影像技术结合时间分辨的质谱技术，研究了3-甲基吡啶分子激发态的超快过程. 实时观察到了3-甲基吡啶分子S₂态向S₁态高振动能级的超快内转换过程，该内转换的时间大约为910fs. 二次布居的S₁态主要通过内转换衰减到基态S₀，该内转换的时间尺度为2.77 ps. 光电子能谱分布和光电子角分布显示，S₂态和S₁态在电离的过程中跟3p里德堡态发生偶然共振. 本次实验中还用400 nm两个光子吸收的方法布居了3-甲基吡啶的3s 里德堡态. 研究表明，3s 里德堡态的寿命为62 fs，并主要通过内转换快速衰减到基态.

关键词:

English

Studies of Ultrafast Dynamics of 3-Picoline with Femtosecond Time-Resolved Photoelectron Imaging

1.
1 Environmental Science and Engineering Research Center, Harbin Institute of Technology Shenzhen Graduate School, Shenzhen 518055, Guangdong Province, P. R. China;
2 State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences, Wuhan 430071, P. R. China;
3 University of Chinese Academy of Sciences, Beijing 100049, P. R. China
Received Date: 29 August 2013
Available Online: 01 January 2014
Fund Project:
国家自然科学基金(91121006，21273274)资助项目

Abstract:

The ultrafast dynamics of excited states in 3-picoline were studied using femtosecond timeresolved photoelectron imaging, coupled with time-resolved mass spectroscopy. An ultrafast internal conversion from the S₂ state to the vibrationally excited S₁ state in about 910 fs was observed. This secondary-populated S₁ state further deactivates to the S₀ state in 2.77 ps. The photoelectron energy and angular distributions show ionizations from the singlet 3p Rydberg states. Two 400 nm photon excitations to the 3s Rydberg state suggest that this state probably decays to the ground state in 62 fs.

Key words:

1. [1]
  
  (1) Crespo-Hernandez, C. E.; Cohen, B.; Hare, P. M.; Kohle, B.Chem. Rev. 2004, 104, 1977. doi: 10.1021/cr0206770
  (1) Crespo-Hernandez, C. E.; Cohen, B.; Hare, P. M.; Kohle, B.Chem. Rev. 2004, 104, 1977. doi: 10.1021/cr0206770
2. [2]
  (2) Middleton, C. T.; Crespo-Hernandez, C. E.; Kohler, B. Annu. Rev. Phys. Chem. 2009, 60, 217. doi: 10.1146/annurev.physchem.59.032607.093719(2) Middleton, C. T.; Crespo-Hernandez, C. E.; Kohler, B. Annu. Rev. Phys. Chem. 2009, 60, 217. doi: 10.1146/annurev.physchem.59.032607.093719
3. [3]
  (3) Stolow, A.; Blanchet, V.; Zgierski, M. Z.; Seideman, T. Nature1999, 401, 52. doi: 10.1038/43410(3) Stolow, A.; Blanchet, V.; Zgierski, M. Z.; Seideman, T. Nature1999, 401, 52. doi: 10.1038/43410
4. [4]
  (4) Schmitt, M.; Lochbrunner, S.; Shaffer, J. P.; Larsen, J. J.;Zgierski, M. Z.; Stolow, A. J. Chem. Phys. 2001, 114, 1206.doi: 10.1063/1.1331637(4) Schmitt, M.; Lochbrunner, S.; Shaffer, J. P.; Larsen, J. J.;Zgierski, M. Z.; Stolow, A. J. Chem. Phys. 2001, 114, 1206.doi: 10.1063/1.1331637
5. [5]
  (5) Suzuki, T.; Whitaker, B. J. Int. Rev. Phys. Chem. 2001, 20, 313.doi: 10.1080/01442350110045046(5) Suzuki, T.; Whitaker, B. J. Int. Rev. Phys. Chem. 2001, 20, 313.doi: 10.1080/01442350110045046
6. [6]
  (6) Suzuki, T.;Wang, L.; Kohguchi, H. J. Chem. Phys. 1999, 111,4859. doi: 10.1063/1.479822(6) Suzuki, T.;Wang, L.; Kohguchi, H. J. Chem. Phys. 1999, 111,4859. doi: 10.1063/1.479822
7. [7]
  (7) Wang, L.; Kohguchi, H.; Suzuki, T. Faraday Discuss. 1999,113, 37. doi: 10.1039/a902866h(7) Wang, L.; Kohguchi, H.; Suzuki, T. Faraday Discuss. 1999,113, 37. doi: 10.1039/a902866h
8. [8]
  (8) Tsubouchi, M.; Whitaker, B. J.;Wang, L.; Kohguchi, H.;Suzuki, T. Phys. Rev. Lett. 2001, 86, 4500. doi: 10.1103/PhysRevLett.86.4500(8) Tsubouchi, M.; Whitaker, B. J.;Wang, L.; Kohguchi, H.;Suzuki, T. Phys. Rev. Lett. 2001, 86, 4500. doi: 10.1103/PhysRevLett.86.4500
9. [9]
  (9) Matsumoto, Y.; Kim, S. K.; Suzuki, T. J. Chem. Phys. 2003,119, 300. doi: 10.1063/1.1578062(9) Matsumoto, Y.; Kim, S. K.; Suzuki, T. J. Chem. Phys. 2003,119, 300. doi: 10.1063/1.1578062
10. [10]
  (10) Oku, M.; Hou, Y.; Xing, X.; Reed, B.; Xu, H.; Chang, C.; Ng,C. Y.; Nishizawa, K.; Ohshimo, K.; Suzuki, T. J. Phys. Chem. A2008, 112, 2293. doi: 10.1021/jp0771466(10) Oku, M.; Hou, Y.; Xing, X.; Reed, B.; Xu, H.; Chang, C.; Ng,C. Y.; Nishizawa, K.; Ohshimo, K.; Suzuki, T. J. Phys. Chem. A2008, 112, 2293. doi: 10.1021/jp0771466
11. [11]
  (11) Suzuki, T.; Tsubouchi, M.;Wang, L. J. Phys. Chem. A 2004,108, 5764.(11) Suzuki, T.; Tsubouchi, M.;Wang, L. J. Phys. Chem. A 2004,108, 5764.
12. [12]
  (12) Abulimiti, B.; Zhu, R. S.; Long, J. Y.; Xu, Y. Q.; Liu, Y. Z.;Ghazal, A. Y.; Yang, M. H.; Zhang, B. J. Chem. Phys. 2011,134, 234301. doi: 10.1063/1.3600334(12) Abulimiti, B.; Zhu, R. S.; Long, J. Y.; Xu, Y. Q.; Liu, Y. Z.;Ghazal, A. Y.; Yang, M. H.; Zhang, B. J. Chem. Phys. 2011,134, 234301. doi: 10.1063/1.3600334
13. [13]
  (13) Chachisvilis, M.; Zewail, A. H. J. Phys. Chem. A 1999, 103,7408. doi: 10.1021/jp991821x(13) Chachisvilis, M.; Zewail, A. H. J. Phys. Chem. A 1999, 103,7408. doi: 10.1021/jp991821x
14. [14]
  (14) Zhong, D. P.; Diau, E.W. G.; Bernhardt, T.; Feyter, S. D.;Roberts, J. D.; Zewail, A. H. Chem. Phys. Lett. 1998, 298,129. doi: 10.1016/S0009-2614(98)01160-9(14) Zhong, D. P.; Diau, E.W. G.; Bernhardt, T.; Feyter, S. D.;Roberts, J. D.; Zewail, A. H. Chem. Phys. Lett. 1998, 298,129. doi: 10.1016/S0009-2614(98)01160-9
15. [15]
  (15) Tsubouchi, M.; Suzuki, T. J. Phys. Chem. A 2003, 107, 10897.doi: 10.1021/jp036333a(15) Tsubouchi, M.; Suzuki, T. J. Phys. Chem. A 2003, 107, 10897.doi: 10.1021/jp036333a
16. [16]
  (16) Roebke,W. J. Phys. Chem. 1970, 74, 4198. doi: 10.1021/j100718a004(16) Roebke,W. J. Phys. Chem. 1970, 74, 4198. doi: 10.1021/j100718a004
17. [17]
  (17) Yamazaki, I.; Baba, H. J. Chem. Phys. 1977, 66, 5826. doi: 10.1063/1.433862(17) Yamazaki, I.; Baba, H. J. Chem. Phys. 1977, 66, 5826. doi: 10.1063/1.433862
18. [18]
  (18) Yamazaki, I.; Sushida, K.; Baba, H. J. Chem. Phys. 1979, 71,381. doi: 10.1063/1.438081(18) Yamazaki, I.; Sushida, K.; Baba, H. J. Chem. Phys. 1979, 71,381. doi: 10.1063/1.438081
19. [19]
  (19) Liu, Y. Z.; Qin, C. C.; Zhang, S.;Wang, Y. M.; Zhang, B. Acta Phys. -Chim. Sin. 2011, 27, 965. [刘玉柱, 秦朝朝, 张嵩,王艳梅, 张冰. 物理化学学报, 2011, 27, 965.] doi: 10.3866/PKU.WHXB20110404(19) Liu, Y. Z.; Qin, C. C.; Zhang, S.;Wang, Y. M.; Zhang, B. Acta Phys. -Chim. Sin. 2011, 27, 965. [刘玉柱, 秦朝朝, 张嵩,王艳梅, 张冰. 物理化学学报, 2011, 27, 965.] doi: 10.3866/PKU.WHXB20110404
20. [20]
  (20) Long, J. Y.; Liu, Y. Z.; Qin, C. C.; Zhang, S.; Zhang, B. Opt. Express 2011, 19, 4542. doi: 10.1364/OE.19.004542(20) Long, J. Y.; Liu, Y. Z.; Qin, C. C.; Zhang, S.; Zhang, B. Opt. Express 2011, 19, 4542. doi: 10.1364/OE.19.004542
21. [21]
  (21) Long, J. Y.; Liu, Y. Z.; Qin, C. C.; Zhang, S.; Zhang, B. Phys. Rev. A 2011, 84, 063409. doi: 10.1103/PhysRevA.84.063409(21) Long, J. Y.; Liu, Y. Z.; Qin, C. C.; Zhang, S.; Zhang, B. Phys. Rev. A 2011, 84, 063409. doi: 10.1103/PhysRevA.84.063409
22. [22]
  (22) Ding, Z. H.; Qiu, X. J.; Xu, Y. Q.;Wang, Y. M.; Zhang, B. Acta Phys. -Chim. Sin. 2012, 28 (12), 2761. [丁中华, 邱学军, 徐晏琪, 王艳梅, 张冰. 物理化学学报, 2012, 28 (12), 2761.] doi: 10.3866/PKU.WHXB201210124(22) Ding, Z. H.; Qiu, X. J.; Xu, Y. Q.;Wang, Y. M.; Zhang, B. Acta Phys. -Chim. Sin. 2012, 28 (12), 2761. [丁中华, 邱学军, 徐晏琪, 王艳梅, 张冰. 物理化学学报, 2012, 28 (12), 2761.] doi: 10.3866/PKU.WHXB201210124
23. [23]
  (23) Dribinski, V.; Ossadtchi, A.; Mandelshtam, V. A.; Reisler, H.Rev. Sci. Instrum. 2002, 73, 2634. doi: 10.1063/1.1482156(23) Dribinski, V.; Ossadtchi, A.; Mandelshtam, V. A.; Reisler, H.Rev. Sci. Instrum. 2002, 73, 2634. doi: 10.1063/1.1482156
24. [24]
  (24) Sreekanth, C. S.; Mok, C. Y.; Huang, H. H. J. Electron Spectrosc. Relat. Phenom. 1991, 56, 105. doi: 10.1016/0368-2048(91)80008-I(24) Sreekanth, C. S.; Mok, C. Y.; Huang, H. H. J. Electron Spectrosc. Relat. Phenom. 1991, 56, 105. doi: 10.1016/0368-2048(91)80008-I
25. [25]
  (25) Suzuki, T. Annu. Rev. Phys. Chem. 2006, 57, 555. doi: 10.1146/annurev.physchem.57.032905.104601(25) Suzuki, T. Annu. Rev. Phys. Chem. 2006, 57, 555. doi: 10.1146/annurev.physchem.57.032905.104601
26. [26]
  (26) Horio, T.; Fuji, T.; Suzuki, Y.; Suzuki, T. J. Am. Chem. Soc.2009, 131, 10392. doi: 10.1021/ja904780b(26) Horio, T.; Fuji, T.; Suzuki, Y.; Suzuki, T. J. Am. Chem. Soc.2009, 131, 10392. doi: 10.1021/ja904780b
27. [27]
  (27) Song, J. K.; Tsubouchi, M.; Suzuki, T. J. Chem. Phys. 2011, 115,8810.(27) Song, J. K.; Tsubouchi, M.; Suzuki, T. J. Chem. Phys. 2011, 115,8810.
28. [28]
  (28) Cao, Z. Z.;Wei, Z. R.; Hua, L. Q.; Hu, C. J.; Zhang, S.; Zhang,B. J. Chem. Phys. 2009, 130, 144309. doi: 10.1063/1.3097184(28) Cao, Z. Z.;Wei, Z. R.; Hua, L. Q.; Hu, C. J.; Zhang, S.; Zhang,B. J. Chem. Phys. 2009, 130, 144309. doi: 10.1063/1.3097184
29. [29]
  (29) Yang, C. N. Phys. Rev. 1948, 74, 764. doi: 10.1103/PhysRev.74.764(29) Yang, C. N. Phys. Rev. 1948, 74, 764. doi: 10.1103/PhysRev.74.764
30. [30]
  (30) Kosmidis, C.; Bolovinos, A.; Tsekeris, P. J. Mol. Spectrosc.1993, 160, 186. doi: 10.1006/jmsp.1993.1167(30) Kosmidis, C.; Bolovinos, A.; Tsekeris, P. J. Mol. Spectrosc.1993, 160, 186. doi: 10.1006/jmsp.1993.1167
31. [31]
  (31) Lee, A. M. D.; Coe, J. D.; Ho, M. L.; Lee, S. J.; Cheng, B. M;Zgierski, M. Z.; Chen, I. C.; Martinez, T. J.; Stolow, A. J. Phys. Chem. A 2007, 111, 11948.
  (31) Lee, A. M. D.; Coe, J. D.; Ho, M. L.; Lee, S. J.; Cheng, B. M;Zgierski, M. Z.; Chen, I. C.; Martinez, T. J.; Stolow, A. J. Phys. Chem. A 2007, 111, 11948.

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

飞秒时间分辨的光电子影像对3-甲基吡啶分子超快动力学研究

English

Studies of Ultrafast Dynamics of 3-Picoline with Femtosecond Time-Resolved Photoelectron Imaging

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

飞秒时间分辨的光电子影像对3-甲基吡啶分子超快动力学研究

English

Studies of Ultrafast Dynamics of 3-Picoline with Femtosecond Time-Resolved Photoelectron Imaging

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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