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129th General Meeting of Korean Chemical Society & Exposition Vibration-mediated valence to non-valence state transition in the ground state of isolated anion

Submission Date :
2 / 27 / 2022 , 18 : 51 : 39
Abstract Number :
129022725948
Presenting Type:
Poster Presentation
Presenting Area :
Physical Chemistry
Authors :
Sejun An, Dabin Kim1, Sang Kyu Kim1,*
Department of Chemistry, KAIST, Korea
1Department of Chemistry, Korea Advanced Institute of Science and Technology, Korea
Assigned Code :
PHYS.P-201 Assigend Code Guideline
Presenting Time :
April 14 (THU) 11:00~13:00

The first observation of electron transfer between the valence to non-valence orbital by the vibrational energy is presented. Dipole-bound state (DBS), one of the non-valence states, is observed after the vibrational excitation with the picosecond-IR laser pulse. A newly constructed cryogenic open-shell anion photoelectron spectrometer was used to observe the valence to non-valence dynamics of the nitromethane anion. By tuning wavelength, we also found out DBS formation yield is maximized when photon energy is resonant to the vibrational frequency of the valence-bound state(VBS), giving new insight into the role of the vibration in the coupling between VBS and DBS. Surprisingly, we also observed that the direct photoemission process forms the DBS, which implies that the photodetached electron is recaptured by the DBS. Our experimental observations regarding electron capturing capability and vibronic coupling mechanism of the DBS support that the non-valence state is a doorway state of electron attachment reaction