Journal
NEW JOURNAL OF PHYSICS
Volume 23, Issue 6, Pages -Publisher
IOP PUBLISHING LTD
DOI: 10.1088/1367-2630/ac0198
Keywords
UV pump-x-ray probe; molecular spectroscopy; ultrafast dynamics; potential energy surfaces; x-ray absorption
Categories
Funding
- RFBR [19-29-12015]
- National Science Foundation of China [11974108, 11574082]
- Fundamental Research Funds for the Central Universities [2021MS046]
- European Union [860553]
- Carl Tryggers Foundation [CTS18:285]
- Helmholtz Virtual Institute [VI419]
- Swedish Research Council [VR 2019-03470, 2018-05973]
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In theoretical simulations, frequency detuning of the pump UV pulse acts as a camera shutter, regulating the duration of the UVX-PP process. A case study on carbon monoxide shows different vibrational profiles in the calculated UVX-PP spectra, revealing details of nuclear dynamics controlled by UV detuning.
In theoretical simulations of a UV + x-ray pump-probe (UVX-PP) setup, we show that frequency detuning of the pump UV pulse acts as a camera shutter by regulating the duration of the UVX-PP process. This two-photon absorption with long overlapping UV and x-ray pulses, allowing for high spectral resolution, thereby provides information about ultrafast dynamics of the nuclear wave packet without the requirement of ultrashort pulses and controlled delay times. In a case study of carbon monoxide, the calculated UVX-PP spectra of the O1s (-1)2 pi (1) and C1s (-1)2 pi (1) core-excited states show different vibrational profiles. The interference of intermediate vibrational states reveals details of nuclear dynamics in the UVX-PP process related to a variable duration time controlled by the UV detuning. Both O1s (-1)2 pi (1) and C1s (-1)2 pi (1) pump-probe channels display a splitting of the spectral profile, which however is associated with different physical mechanisms. At the O1s (-1)2 pi (1) resonance, the observed dispersive and non-dispersive spectral bands intersect and result in destructive interference.
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