Shake-Down Spectroscopy as State- and Site-Specific Probe of Ultrafast Chemical Dynamics

We demonstrate that X-ray pulses from a seeded FEL enable the measurement of high-resolution, time-resolved X-ray photoelectron spectra that capture weak satellite states resulting from shake-down processes in a valence-excited CS2 molecule. H.J.Thompson et al. JACS 147, 32851(2025)
 





We report the first time-resolved observation of shake-down transitions from laser-excited CS2 molecules probed above the S 2p edge with FEL radiation. The satellite states, in particular, provide a sensitive and selective probe of the electronic and geometric structure changes that occur over the course of a photochemical reaction.
 


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Thompson H.J., Bonanomi M., Pedersen J., Plekan O., Pal N., Grazioli C., Prince K.C., Tenorio B.N.C., Devetta M., Faccialà D., Vozzi C., Piseri P., Danailov M.B., Demidovich A., Brynes A.D., Simoncig A., Zangrando M., Coreno M., Feifel R., Squibb R.J., Holland D.M.P., Allum F., Rolles D., Decleva P., Schuurman M.S., Forbes R., Coriani S., Callegari C., Minns R.S., Di Fraia M. (doi: 10.1021/jacs.5c09162)
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