Excited-state reaction dynamics of the radical anions revealed by time-resolved photofragment depletion spectroscopy

Sejun An and Sang Kyu Kim ()
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Sejun An: KAIST
Sang Kyu Kim: KAIST

Nature Communications, 2025, vol. 16, issue 1, 1-7

Abstract: Abstract The excited-state reaction dynamics of radical anions are investigated using a newly developed technique: time-resolved photofragment depletion spectroscopy. This method leverages differences in photodetachment cross-sections among transient anionic species involved in the reaction pathway. It offers a distinct advantage for studying radical anions, which are typically challenging to probe using conventional spectroscopic techniques due to their low electron affinities. As a benchmark, the method is first applied to I₂⁻, whose excited-state behavior is well characterized. The technique is then extended to CH₃NO₂⁻ and (CH₃NO₂)₂⁻, enabling real-time probing of the excited-state dynamics of their nonvalence-bound states. Our findings reveal that ultrafast internal conversion from a nonvalence orbital to a valence orbital is followed either by prompt chemical bond dissociation or by comparatively slower cluster decomposition. These results highlight the dynamic role of the nonvalence orbital in driving chemical reactivity.

Date: 2025
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DOI: 10.1038/s41467-025-61295-y

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