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Resonant inelastic x-ray scattering reveals hidden local transitions of the aqueous OH radical

Kjellsson, L., Nanda, K. D., Rubensson, J. E., Doumy, G., Southworth, S. H., Ho, P. J., March, A. M., Al Haddad, A., Kumagai, Y., Tu, M. F., Schaller, R. D., Debnath, T., Bin Mohd Yusof, M. S., Arnold, C., Schlotter, W. F., Moeller, S., Coslovich, G., Koralek, J. D., Minitti, M. P., Vidal, M. L., Simon, M., Santra, R., Loh, Z.-H., Coriani, S., Krylov, A. I. and Young, L. 2020. Resonant inelastic x-ray scattering reveals hidden local transitions of the aqueous OH radical. Physical Review Letters 124 (23) , 236001. 10.1103/PhysRevLett.124.236001

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Resonant inelastic x-ray scattering (RIXS) provides remarkable opportunities to interrogate ultrafast dynamics in liquids. Here we use RIXS to study the fundamentally and practically important hydroxyl radical in liquid water, OH(aq). Impulsive ionization of pure liquid water produced a short-lived population of OH(aq), which was probed using femtosecond x-rays from an x-ray free-electron laser. We find that RIXS reveals localized electronic transitions that are masked in the ultraviolet absorption spectrum by strong charge-transfer transitions—thus providing a means to investigate the evolving electronic structure and reactivity of the hydroxyl radical in aqueous and heterogeneous environments. First-principles calculations provide interpretation of the main spectral features.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Publisher: American Physical Society
ISSN: 0031-9007
Date of Acceptance: 22 May 2020
Last Modified: 20 May 2021 15:30

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