TY - JOUR
AU - Gabalski, Ian
AU - Allum, Felix
AU - Seidu, Issaka
AU - Britton, Mathew
AU - Brenner, Guenter
AU - Bromberger, Hubertus
AU - Brouard, Mark
AU - Bucksbaum, Philip
AU - Burt, Michael
AU - Cryan, James
AU - Driver, Taran
AU - Ekanayake, Nagitha
AU - Erk, Benjamin
AU - Garg, Diksha
AU - Gougoula, Eva
AU - Heathcote, David
AU - Hockett, Paul
AU - Holland, David
AU - Howard, Andrew
AU - Kumar, Sonu
AU - Lee, Jason Wai Lung
AU - Li, Siqi
AU - McManus, Joseph
AU - Mikosch, Jochen
AU - Milesevic, Dennis
AU - Minns, Russell
AU - Neville, Simon
AU - Atia-Tul-Noor
AU - Papadopoulou, Christina
AU - Passow, Christopher
AU - Razmus, Weronika
AU - Roeder, Anja
AU - Rouzee, Arnaud
AU - Pinto Simao, Alcides
AU - Unwin, James
AU - Vallance, Claire
AU - Walmsley, Tiffany
AU - Wang, Jun
AU - Rolles, Daniel
AU - Stolow, Albert
AU - Schuurman, Michael
AU - Forbes, Ruaridh
TI - Time-Resolved X-ray Photoelectron Spectroscopy: Ultrafast Dynamics in CS<sub>2</sub> Probed at the S 2p Edge
JO - The journal of physical chemistry letters
VL - 14
IS - 31
SN - 1948-7185
CY - Washington, DC
PB - ACS
M1 - PUBDB-2023-05122
SP - 7126 - 7133
PY - 2023
AB - Recent developments in X-ray free-electron lasers have enabled a novel site-selective probe of coupled nuclear and electronic dynamics in photoexcited molecules, time-resolved X-ray photoelectron spectroscopy (TRXPS). We present results from a joint experimental and theoretical TRXPS study of the well-characterized ultraviolet photodissociation of CS2, a prototypical system for understanding non-adiabatic dynamics. These results demonstrate that the sulfur 2p binding energy is sensitive to changes in the nuclear structure following photoexcitation, which ultimately leads to dissociation into CS and S photoproducts. We are able to assign the main X-ray spectroscopic features to the CS and S products via comparison to a first-principles determination of the TRXPS based on ab initio multiple-spawning simulations. Our results demonstrate the use of TRXPS as a local probe of complex ultrafast photodissociation dynamics involving multimodal vibrational coupling, nonradiative transitions between electronic states, and multiple final product channels.
LB - PUB:(DE-HGF)16
C6 - 37534743
UR - <Go to ISI:>//WOS:001042105300001
DO - DOI:10.1021/acs.jpclett.3c01447
UR - https://bib-pubdb1.desy.de/record/589257
ER -