WIPM OpenIR
Excited state dynamics of molecules studied with femtosecond time-resolved mass spectrometry and photoelectron imaging
Wang Yan-Mei1,2; Tang Ying1,2; Zhang Song1,2; Long Jin-You1,2; Zhang Bing1,2
2018-11-20
Source PublicationACTA PHYSICA SINICA
ISSN1000-3290
Volume67Issue:22Pages:16
AbstractStudy 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 S-1 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 pi 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.
Keywordfemtosecond time-resolved mass spectrometry photoelectron imaging dynamics in excited states
Funding OrganizationNational Natural Science Foundation of China ; National Natural Science Foundation of China ; National Basic Research Program of China ; National Basic Research Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Basic Research Program of China ; National Basic Research Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Basic Research Program of China ; National Basic Research Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Basic Research Program of China ; National Basic Research Program of China
DOI10.7498/aps.67.20181334
WOS KeywordULTRAFAST INTERNAL-CONVERSION ; KINETIC-ENERGY PHOTOELECTRON ; SUB-DOPPLER SPECTROSCOPY ; WAVE-PACKET ; ROTATIONAL COHERENCE ; PUMP-PROBE ; FRACTIONAL REVIVALS ; MULTIREFERENCE CALCULATIONS ; PHOTODISSOCIATION DYNAMICS ; IONIZATION SPECTROSCOPY
Language英语
Funding ProjectNational Natural Science Foundation of China[21573279] ; National Natural Science Foundation of China[11574351] ; National Natural Science Foundation of China[11674355] ; National Natural Science Foundation of China[21303255] ; National Natural Science Foundation of China[91121006] ; National Natural Science Foundation of China[21273274] ; National Natural Science Foundation of China[21773299] ; National Basic Research Program of China[2013CB922200]
Funding OrganizationNational Natural Science Foundation of China ; National Natural Science Foundation of China ; National Basic Research Program of China ; National Basic Research Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Basic Research Program of China ; National Basic Research Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Basic Research Program of China ; National Basic Research Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Basic Research Program of China ; National Basic Research Program of China
WOS Research AreaPhysics
WOS SubjectPhysics, Multidisciplinary
WOS IDWOS:000455402400034
PublisherCHINESE PHYSICAL SOC
Citation statistics
Document Type期刊论文
Identifierhttp://ir.wipm.ac.cn/handle/112942/14145
Collection中国科学院武汉物理与数学研究所
Corresponding AuthorZhang Bing
Affiliation1.Chinese Acad Sci, Wuhan Inst Phys & Math, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan 430071, Hubei, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
Recommended Citation
GB/T 7714
Wang Yan-Mei,Tang Ying,Zhang Song,et al. Excited state dynamics of molecules studied with femtosecond time-resolved mass spectrometry and photoelectron imaging[J]. ACTA PHYSICA SINICA,2018,67(22):16.
APA Wang Yan-Mei,Tang Ying,Zhang Song,Long Jin-You,&Zhang Bing.(2018).Excited state dynamics of molecules studied with femtosecond time-resolved mass spectrometry and photoelectron imaging.ACTA PHYSICA SINICA,67(22),16.
MLA Wang Yan-Mei,et al."Excited state dynamics of molecules studied with femtosecond time-resolved mass spectrometry and photoelectron imaging".ACTA PHYSICA SINICA 67.22(2018):16.
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