Intersystem crossing of 2-Methlypyrazine studied by femtosecond photoelectron imaging

Bumaliya Abulimiti; Ling Feng-Zi; Deng Xu-Lan; Wei Jie; Song Xin-Li; Xiang Mei; Zhang Bing

doi:10.7498/aps.69.20200092

Abstract

The ultrafast nonadibatic relaxation dynamics of the excited state of 2-methylpyrazine has been studied by using femtosecond time-resolved photoelectron imaging and femtosecond time-resolved mass spectrometry. The first excited state S₁ of 2-methylpyrazine was excited by 323 nm pump light, and the excited state deactivation process is detected by 400 nm probe light. The lifetime of S₁ state 98 ps is obtained by time-resolved mass spectroscopy. The intersystem crossing from the S₁ state to the T₁ state is observed on real time. The relaxation dynamics of S₁ state of 2-methlypyrazine is different from that of pyrazine, the results show that the intersystem crossing process between S₁ and T₁ is the main relaxation channel of S₁ state of 2-methlypyrazine, but the internal conversion process between S₁ and S₀ is also a main relaxation channel of S₁ state. By using the advantages of femtosecond time-resolved photoelectron imaging, the photoelectron angular distribution at different pump-probe time delay was obtained experimentally. From the photoelectron angle distribution combined with photoelectron kinetic energy distributions, we tried to observe the field-free nonadiabatic alignment. However, due to the fact that the molecular symmetry of 2-methylpyrazine is lower than that of pyrazine, it is more challenging to observe the phenomenon of molecular nonadiabatic alignment with lower symmetry. Therefore, it is fail to observe nonadiabatic alignment feature of 2-methylpyrazine in this experiment. This work provides a clearer physical picture for S₁ state nonadibatic relaxation dynamics of 2-methylpyrazine.

Keywords:

Authors and contacts

1.
College of Physics and Electronic Engineering, Xinjiang Normal University, Urumqi 830054, 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, China

Corresponding author: Bumaliya Abulimiti, maryam917@163.com ; Xiang Mei, xm120922@xjnu.edu.cn ;

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References

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图 1 (a)光电子影像装置实物图; (b)飞秒时间分辨光电子影像装置示意图^[21]

Figure 1. (a) Photoelectron imaging apparatus; (b) schematic diagram of the femtosecond time resolved photoelectron imaging setup.

DownLoad: Full-Size Img PowerPoint

图 2 (a)泵浦光323 nm, 探测光400 nm的各自单光和零时刻双光质谱;(b)泵浦光323 nm, 探测光400 nm作用下时间分辨母体离子信号, 图中实线表示拟合曲线, 圆圈代表实验数据

Figure 2. (a) Two color (at time overlap) and one color mass spectra of 2-methlypyrazine at 323 nm pump and 400 nm probe; (b) time-resolved total ion signals of parent ion as a function of delay time between the pump pulse at 323 nm and the probe pulse at 400 nm. The circles are the experimental results, and solid lines are the fitting results.

DownLoad: Full-Size Img PowerPoint

图 3 泵浦光323 nm, 探测光400 nm, 在不同时间延迟下的光电子原始影像和BASEX变换后的影像(上排为原始影像, 而下排为BASEX变换后的影像.). 泵浦光和探测光都是线偏振光, 偏振方向为图平面竖直方向

Figure 3. Time-resolved photoelectron raw images (shown in the upper row) and BASEX-inverted images (shown in the lower row) at various time delays observed at 323 nm pump and 400 nm probe.

DownLoad: Full-Size Img PowerPoint

图 4 (a)不同延迟时间下的光电子能谱; (b) 0 fs和92 ps时的光电子能谱

Figure 4. (a) Photoelectron kinetic energy distributions (PKE) at different time delay; (b) photoelectron kinetic energy distributions at 0 and 92 ps.

DownLoad: Full-Size Img PowerPoint

图 5 六个峰强度随泵浦-探测时间变化图

Figure 5. Time-resolved PKE bands intensity as a function of representative delay times.

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图 6 (a) 0—4 ps泵浦-探测时间延迟下不同光电子峰强度变化; (b)不同光电子峰对应的不同泵浦-探测时间延迟下各向异性参数

Figure 6. (a) The intensity changes of different photoelectronic peaks with 0–4 ps pump- probe time delay; (b) anisotropy parameters of the six rings as a function of pump-probe time delay.

DownLoad: Full-Size Img PowerPoint

图 7 (a) 105—130 ps泵浦-探测时间延迟下不同光电子峰强度变化; (b)不同光电子峰对应不同泵浦-探测时间延迟下的各向异性参数

Figure 7. (a) The intensity changes of different photoelectronic peaks with 105–130 ps pump- probe time delay; (b) anisotropy parameters of the six rings as a function of pump-probe time delay.

DownLoad: Full-Size Img PowerPoint

图 8 2-甲基吡嗪分子被323 nm泵浦400 nm探测下的跃迁和电离机理示意图

Figure 8. Schematic representation of the excitation and ionization scheme of 2-methlypyrazine using 323 nm pump and 400 nm probe pulses.

DownLoad: Full-Size Img PowerPoint

map

[1]	De Gruijl F 1999 Eur. J. Cancer 35 2003 Google Scholar
[2]	Ichihashi M, Ueda M, Budiyanto A, Bito T, Oka M, Fukunaga M, Tsuru K, Horikawa T 2003 Toxicology 189 21 Google Scholar
[3]	Iqbal A, Stavros V G 2010 J. Phys. Chem. Lett. 1 2274 Google Scholar
[4]	Domcke W, Stock G 1997 Adv. Chem. Phys. 100 1
[5]	Gustavsson T, Improta R, Markovitsi D 2010 J. Phys. Chem. Lett. 1 2025 Google Scholar
[6]	Schoenlein R W, Peteanu L A, Mathies R, Shank C V 1991 Science 254 412 Google Scholar
[7]	Suzuki T, Wang L, Kohguchi H 1999 J. Chem. Phys. 111 4859 Google Scholar
[8]	Song J K, Tsubouchi M, Suzuki T 2001 J. Chem. Phys. 115 8810 Google Scholar
[9]	Ling F Z, Li S, Song X L, Wang Y M, Long J Y, Zhang B 2017 Sci. Rep. 7 15362 Google Scholar
[10]	Toshinori S 2014 Bull. Chem. Soc. Jpn. 87 341 Google Scholar
[11]	Farmanara P, Stert V, Radloff W, Hertel I V 2001 J. Phys. Chem. A 105 5613 Google Scholar
[12]	Suzuki Y I, Horio T, Fuji T, Suzuki T 2011 J. Chem. Phys. 134 184313 Google Scholar
[13]	Frad A, Lahmani F, Tramer A, Tric C 1974 J. Chem. Phys. 60 4419 Google Scholar
[14]	Zhong D, Diau E W G, Bernhardt T M, Feyter S D, Roberts J D, Zewail A H 1998 Chem. Phys. Lett. 298 129 Google Scholar
[15]	Wang L, Kohguchi H, Suzuki T 1999 Faraday Discuss. 113 37 Google Scholar
[16]	Tsubouchi M, Whitaker B J, Wang L, Kohguchi H, Suzuki T 2001 Phys. Rev. Lett. 86 4500 Google Scholar
[17]	刘玉柱, 肖韶荣, 王俊锋, 何仲福, 邱学军, Gregor Knopp 2016 65 113301 Google Scholar Liu Y Z, Xiao S R, Wang J F, He Zhong F, Qiu X J, Knopp G 2016 Acta Phys. Sin. 65 113301 Google Scholar
[18]	刘玉柱, 陈云云, 郑改革, 金峰Gregor, Knopp 2016 65 053302 Google Scholar Liu Y Z, Chen Y Y, Zheng G G, Jin F, Knopp G 2016 Acta Phys. Sin. 65 053302 Google Scholar
[19]	Liu Y Z, Knopp G, Qin C C, Gerber T 2015 Chem. Phys. 446 142 Google Scholar
[20]	Fuji T, Suzuki Y I, Horio T, Suzuki T, Mitrić R, Werner U, Koutecký V B 2010 J. Chem. Phys. 133 234303 Google Scholar
[21]	凌丰姿 2018 博士学位论文(武汉: 中国科学院武汉物理与数学研究所) Ling F Z 2018 Ph. D. Dissertation (Wuhan: Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences) (in Chinese)
[22]	Hao Q L, Long J Y, Deng X L, Tang Y, Abulimiti B, Zhang B 2017 J. Phys. Chem. A 121 3858 Google Scholar
[23]	Ling F, Li S, Wei J, Liu K, Wang Y M, Zhang B 2018 J. Chem. Phys. 148 144311 Google Scholar
[24]	Dribinski V, Ossadtchi A, Mandelshtam V. A, Reisler H 2002 Rev. Sci. Instrum. 73 2634 Google Scholar
[25]	Matsumoto Y, Kim S. K, Suzuki T 2003 J. Chem. Phys. 119 300 Google Scholar

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