| Author | Search for: Schuurman, Michael S.1 |
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| Affiliation | - National Research Council of Canada. Security and Disruptive Technologies
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| Format | Text, Abstract |
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| Conference | 53rd Annual Meeting of the APS Division of Atomic, Molecular and Optical Physics, May 30 – June 3 2022, Orlando, FL, USA |
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| Abstract | Developments in ultrafast X-ray sources offer powerful new means of probing the complex nonadiabatic dynamics in photoexcited molecules. Of particular interest are the electronic and nuclear structures associated with conical intersections, which are predicted to have unique spectral signatures when probed using X-ray spectroscopies. Using high level ab initio quantum dynamics simulations and newly developed electronic structure techniques based on the DFT/MRCI formalism, we have simulated time-resolved X-ray spectroscopy (TRXAS and TRXPS) of a number of prototypical unsaturated organic chromophores. These spectroscopies are sensitive to all aspects of the ensuing dynamics and can distinguish between the different nuclear dynamical pathways that result in electronic relaxation. The ability of femtosecond X-ray spectroscopy to provide a clear picture of the wave packet dynamics near conical intersections is related to transient charge localization at specific atomic sites that is driven by the nuclear dynamics. These dramatic changes in the local charge environment are then 'reported' using the core-electrons localized on, or proximate to, the atoms involved in the formation of these transient electronic structures. Given the complexity of the measured signals, and the difficulty in empirically (and uniquely) mapping transient spectra to molecular structures, the role of accurate simulations will be essential for the interpretation of these new time-resolved spectroscopies. |
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| Publication date | 2022-05-30 |
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| Publisher | American Physical Society |
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| In | |
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| Language | English |
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| Export citation | Export as RIS |
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| Report a correction | Report a correction (opens in a new tab) |
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| Record identifier | f507a285-4549-4ebd-b1fc-39e29ac4857d |
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| Record created | 2023-05-04 |
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| Record modified | 2024-04-09 |
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