Excited state dynamics of molecules studied with femtosecond time-resolved mass spectrometry and photoelectron imaging

Wang Yan-Mei; Tang Ying; Zhang Song; Long Jin-You; Zhang Bing

doi:10.7498/aps.67.20181334

Abstract

Study of quantum states of molecules, especially the evolution of excited states can help to understand their basic features and the interactions among different states. Furthermore, the information about the chemical reaction process and the interactions among several reaction channels can be obtained. Femtosecond time-resolved mass spectrometry (TRMS) and time-resolved photoelectron imaging (TRPEI), which combine pump-probe technique with time of flight mass spectrometry and photoelectron imaging, are powerful tools for detecting the molecular quantum state and for studying the molecular quantum state interaction and molecular ultrafast dynamics. With these methods, the photochemistry and photophysics mechanism of isolated molecule reaction process can be investigated on a femtosecond time scale. The principles of TRMS and TRPEI are introduced here in detail. On the basis of substantial research achievements in our group, the applications of TRMS and TRPEI are presented in the study of ultrafast internal conversion and intersystem crossing, wavepacket evolution dynamics at excited states of polyatomic molecules, energy transfer process of polyatomic molecules, ultrafast photodissociation dynamics and structural evolution dynamics of molecular excited states. In the study of ultrafast internal conversion and intersystem crossing, the methyl substituted benzene derivatives and benzene halides are discussed as typical molecular systems. In the study of wavepacket evolution dynamics at excited states of polyatomic molecules, the real-time visualization of the dynamic evolution of CS2 4d and 6s Rydberg wave packet components, the vibrational wave packet dynamics in electronically excited pyrimidine, the rotational wave packet revivals and field-free alignment in excited o-dichlorobenzene are reported. In order to discuss the energy transfer process of polyatomic molecules, the intramolecular vibrational energy redisctribution between different vibrational states in p-difluorobenzene in the S1 low-energy regime and the intramolecular energy transfer between different electronic states in excited cyclopentanone are presented. For the study of ultrafast photodissociation dynamics, the dissociation constants and dynamics of the A band and even higher Rydberg states are investigated for the iodine alkanes and iodine cycloalkanes. Structural evolution dynamics of molecular excited states is the main focus of our recent research. The structural evolution dynamics can be extracted from the coherent superposition preparation of quantum states and the observation of quantum beat phenomenon, by taking 2, 4-difluorophenol and o-fluorophenol as examples. Time-dependent photoelectron peaks originating from the planar and nonplanar geometries in the first excited state in 2, 4-difluorophenol exhibit the clear beats with similar periodicities but a phase shift of π rad, offering an unambiguous picture of the oscillating nuclear motion between the planar geometry and the nonplanar minimum. Also, the structural evolution dynamics in o-fluorophenol via the butterfly vibration between planar geometry and nonplanar minimum is mapped directly. Finally, the potential developments and further possible research work and future directions of these techniques and researches are prospected.

Keywords:

Authors and contacts

1.
State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences, Wuhan 430071, China;
2.
University of Chinese Academy of Sciences, Beijing 100049, China

Corresponding author: Zhang Bing, bzhang@wipm.ac.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 21573279, 11574351, 11674355, 21303255, 91121006, 21273274, 21773299) and the National Basic Research Program of China (Grant No. 2013CB922200).

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Cited By

[1]	Zewail A H 2000 J. Phys. Chem. A 104 5660
[2]	Bixon M, Jortner J 1968 J. Chem. Phys. 48 715
[3]	Jortner J, Rice S A, Hochstrasser R M 1969 Adv. Photochem. 7 149
[4]	Henry S R, Siebrand W 1973 Organic Molecular Photophysics (Vol. 1) (London: Wiley) p152
[5]	Freed K F 1976 Radiationless Processes in Molecules and Condensed Phases (Berlin: Springer-Verlag) p23
[6]	Stock G, Domche W 1997 Adv. Phys. Chem. 100 1
[7]	Michl J, Bonacic-Koutechy V 1990 Electronic Aspects of Organic Photochemistry (New York: Wiley) p284
[8]	Schoenlein R W, Peteanu L A, Mathies R A, Shank C V 1991 Science 254 412
[9]	Jortner J, Ratner M A 1997 Molecular Electronics (Oxford: Blackwell) p5
[10]	Berera R, van Grondelle R, Kennis J T M 2009 Photosynth. Res. 101 105
[11]	Ruckebusch C, Sliwa M, Pernot P, de Juan A, Tauler R 2012 J. Photoch. Photobiol. C 13 1
[12]	Murti Y, Vijayan C 2014 Essentials of Nonlinear Optics (Chapter 5) (Chichester: Wiley & Sons) p77
[13]	Zewail A H 1988 Science 242 1645
[14]	Willberg D M, Breen J J, Gutmann M, Zewail A H 1991 J. Chem. Phys. 95 7136
[15]	Ashfold M N R, Howe J D 1994 Annu. Rev. Phys. Chem. 45 57
[16]	Urban P L, Chen Y C, Wang Y S 2016 Time-Resolved Mass Spectrometry: From Concept to Applications (Chichester: Wiley) p5
[17]	Chen Y C, Urban P L 2013 TrAC Trends Anal. Chem. 44 106
[18]	Suzuki T 2006 Annu. Rev. Phys. Chem. 57 555
[19]	Suzuki T 2012 Int. Rev. Phys. Chem. 31 265
[20]	Pedersen S, Herek J L, Zewail A H 1994 Science 266 1359
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[40]	Yang D, Chen Z, He Z, Wang H, Min Y, Yuan K, Dai D, Wu G, Yang X 2017 Phys. Chem. Chem. Phys. 19 29146
[41]	Yang D, Min Y, Chen Z, He Z, Yuan K, Dai D, Yang X, Wu G 2018 Phys. Chem. Chem. Phys. 20 15015
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