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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
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KCS