Time-dependent nonequilibrium soft x-ray response during a spin crossover
Abstract
Here, the rapid development of high-brilliance pulsed X-ray sources with femtosecond time resolution has created a need for a better theoretical understanding of the time-dependent soft-X-ray response of dissipative many-body quantum systems. It is demonstrated how soft-X-ray spectroscopies, such as X-ray absorption and resonant inelastic X-ray scattering at transition-metal L-edges, can provide insight into intersystem crossings, such as a spin crossover. The photoinduced doublet-to-quartet spin crossover on cobalt in Fe-Co Prussian blue analogues is used as an example to demonstrate how the X-ray response is affected by the dissipative nonequilibrium dynamics. The time-dependent soft-X-ray spectra provide a wealth of information that reflect the changes in the nonequilibrium initial state via continuously changing spectral lineshapes that cannot be decomposed into initial photoexcited and final metastable spectra, strong broadenings, a collapse of clear selection rules during the intersystem crossing, strong fluctuations in the isotropic branching ratio in X-ray absorption, and crystal-field collapse/oscillations and strongly time-dependent anti-Stokes processes in RIXS.
- Authors:
-
- Northern Illinois Univ., DeKalb, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1431228
- Alternate Identifier(s):
- OSTI ID: 1424814
- Grant/Contract Number:
- AC02-06CH11357; FG02-03ER46097
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 97; Journal Issue: 12; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS
Citation Formats
van Veenendaal, Michel. Time-dependent nonequilibrium soft x-ray response during a spin crossover. United States: N. p., 2018.
Web. doi:10.1103/physrevb.97.125108.
van Veenendaal, Michel. Time-dependent nonequilibrium soft x-ray response during a spin crossover. United States. https://doi.org/10.1103/physrevb.97.125108
van Veenendaal, Michel. Thu .
"Time-dependent nonequilibrium soft x-ray response during a spin crossover". United States. https://doi.org/10.1103/physrevb.97.125108. https://www.osti.gov/servlets/purl/1431228.
@article{osti_1431228,
title = {Time-dependent nonequilibrium soft x-ray response during a spin crossover},
author = {van Veenendaal, Michel},
abstractNote = {Here, the rapid development of high-brilliance pulsed X-ray sources with femtosecond time resolution has created a need for a better theoretical understanding of the time-dependent soft-X-ray response of dissipative many-body quantum systems. It is demonstrated how soft-X-ray spectroscopies, such as X-ray absorption and resonant inelastic X-ray scattering at transition-metal L-edges, can provide insight into intersystem crossings, such as a spin crossover. The photoinduced doublet-to-quartet spin crossover on cobalt in Fe-Co Prussian blue analogues is used as an example to demonstrate how the X-ray response is affected by the dissipative nonequilibrium dynamics. The time-dependent soft-X-ray spectra provide a wealth of information that reflect the changes in the nonequilibrium initial state via continuously changing spectral lineshapes that cannot be decomposed into initial photoexcited and final metastable spectra, strong broadenings, a collapse of clear selection rules during the intersystem crossing, strong fluctuations in the isotropic branching ratio in X-ray absorption, and crystal-field collapse/oscillations and strongly time-dependent anti-Stokes processes in RIXS.},
doi = {10.1103/physrevb.97.125108},
journal = {Physical Review B},
number = 12,
volume = 97,
place = {United States},
year = {Thu Mar 08 00:00:00 EST 2018},
month = {Thu Mar 08 00:00:00 EST 2018}
}
Web of Science
Figures / Tables:
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Works referencing / citing this record:
Dissipation and dynamics in ultrafast intersystem crossings
journal, January 2020
- van Veenendaal, Michel
- The Journal of Chemical Physics, Vol. 152, Issue 2
Figures / Tables found in this record: