Characterizing coherences in chemical dynamics with attosecond time-resolved x-ray absorption spectroscopy
Abstract
Coherence can drive wave-like motion of electrons and nuclei in photoexcited systems, which can yield fast and efficient ways to exert materials’ functionalities beyond the thermodynamic limit. The search for coherent phenomena has been a central topic in chemical physics although their direct characterization is often elusive. Here, we highlight recent advances in time-resolved x-ray absorption spectroscopy (tr-XAS) to investigate coherent phenomena, especially those that utilize the eminent light source of isolated attosecond pulses. The unparalleled time and state sensitivities of tr-XAS in tandem with the unique element specificity render the method suitable to study valence electronic dynamics in a wide variety of materials. The latest studies have demonstrated the capabilities of tr-XAS to characterize coupled electronic–structural coherence in small molecules and coherent light–matter interactions of core-excited excitons in solids. We address current opportunities and challenges in the exploration of coherent phenomena, with potential applications for energy- and bio-related systems, potential crossings, strongly driven solids, and quantum materials, and so with the ongoing developments in both theory and light sources, tr-XAS holds great promise for revealing the role of coherences in chemical dynamics.
- Authors:
-
- SLAC National Accelerator Laboratory, Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); Stanford University, CA (United States); University of California, Berkeley, CA (United States)
- University of California, Berkeley, CA (United States):Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; US Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF); Stanford University; USDOE
- OSTI Identifier:
- 1908925
- Alternate Identifier(s):
- OSTI ID: 1897585
- Grant/Contract Number:
- AC02-76SF00515; AC02-05CH11231; FA9550-19-1-0314; FA9550-20-1-0334; CHE-1951317
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 157; Journal Issue: 18; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Kobayashi, Yuki, and Leone, Stephen R. Characterizing coherences in chemical dynamics with attosecond time-resolved x-ray absorption spectroscopy. United States: N. p., 2022.
Web. doi:10.1063/5.0119942.
Kobayashi, Yuki, & Leone, Stephen R. Characterizing coherences in chemical dynamics with attosecond time-resolved x-ray absorption spectroscopy. United States. https://doi.org/10.1063/5.0119942
Kobayashi, Yuki, and Leone, Stephen R. Tue .
"Characterizing coherences in chemical dynamics with attosecond time-resolved x-ray absorption spectroscopy". United States. https://doi.org/10.1063/5.0119942. https://www.osti.gov/servlets/purl/1908925.
@article{osti_1908925,
title = {Characterizing coherences in chemical dynamics with attosecond time-resolved x-ray absorption spectroscopy},
author = {Kobayashi, Yuki and Leone, Stephen R.},
abstractNote = {Coherence can drive wave-like motion of electrons and nuclei in photoexcited systems, which can yield fast and efficient ways to exert materials’ functionalities beyond the thermodynamic limit. The search for coherent phenomena has been a central topic in chemical physics although their direct characterization is often elusive. Here, we highlight recent advances in time-resolved x-ray absorption spectroscopy (tr-XAS) to investigate coherent phenomena, especially those that utilize the eminent light source of isolated attosecond pulses. The unparalleled time and state sensitivities of tr-XAS in tandem with the unique element specificity render the method suitable to study valence electronic dynamics in a wide variety of materials. The latest studies have demonstrated the capabilities of tr-XAS to characterize coupled electronic–structural coherence in small molecules and coherent light–matter interactions of core-excited excitons in solids. We address current opportunities and challenges in the exploration of coherent phenomena, with potential applications for energy- and bio-related systems, potential crossings, strongly driven solids, and quantum materials, and so with the ongoing developments in both theory and light sources, tr-XAS holds great promise for revealing the role of coherences in chemical dynamics.},
doi = {10.1063/5.0119942},
journal = {Journal of Chemical Physics},
number = 18,
volume = 157,
place = {United States},
year = {Tue Nov 08 00:00:00 EST 2022},
month = {Tue Nov 08 00:00:00 EST 2022}
}
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