Journal
PHYSICAL REVIEW X
Volume 11, Issue 3, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevX.11.031001
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Funding
- European Research Council (ERC) [X-MuSiC-616783]
- Ministry of Education, Singapore [RG105/17, RG1/20]
- DFG through QUTIF Priority Programme
- Division of Chemical Sciences, Geosciences, and Biosciences of the U.S. Department of Energy at LBNL [DEAC02-05CH11231]
- National Science Foundation [CHE-1660417]
- BMBF [05K13PM2]
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In this study, an extreme-ultraviolet free-electron laser is used to excite a gas-phase di-iodomethane target, allowing for the investigation of molecular dissociation pathways and geometries in a time-resolved manner. The method presented in this work provides a sensitive approach to study excited-state molecular structures and reactions triggered by core-resonance at specific sites.
In this work, we use an extreme-ultraviolet (XUV) free-electron laser (FEL) to resonantly excite the I:4d(5/2)(-sigma*) transition of a gas-phase di-iodomethane (CH2I2) target. This site-specific excitation generates a 4d core hole located at an iodine site, which leaves the molecule in a well-defined excited state. We subsequently measure the time-dependent absorption change of the molecule with the FEL probe spectrum centered on the same I: 4d resonance. Using ab initio calculations of absorption spectra of a transient isomerization pathway observed in earlier studies, our time-resolved measurements allow us to assign the timescales of the previously reported direct and indirect dissociation pathways. The presented method is thus sensitive to excited-state molecular geometries in a time-resolved manner, following a core-resonant site-specific trigger.
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