Demonstration of resonant inelastic x-ray scattering as a probe of exciton-phonon coupling
Abstract
Resonant inelastic x-ray scattering (RIXS) is a promising technique for obtaining electron-phonon coupling constants. However, the ability to extract these coupling constants throughout the Brillouin zone for crystalline materials remains limited. To address this need, we developed a Green's function formalism to capture electron-phonon contributions to core-level spectroscopies without explicitly solving the full vibronic problem. Our approach is based on the cumulant expansion of the Green's function combined with many-body theory calculated vibrational coupling constants. The methodology is applied to x-ray photoemission spectroscopy, x-ray absorption spectroscopy (XAS), and RIXS. In the case of the XAS and RIXS, we use a two-particle exciton Green's function, which accounts implicitly for particle-hole interference effects that have previously proved difficult. To demonstrate the methodology and gain a deeper understanding of the experimental technique, we apply our formalism to small molecules, for which unambiguous experimental data exist. This comparison reveals that the vibronic coupling constant probed by RIXS is in fact related to exciton-phonon coupling rather than electron-phonon coupling, challenging the conventional interpretation of the experiment.
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1637655
- Report Number(s):
- BNL-216122-2020-JAAM
Journal ID: ISSN 2469-9950;2469-9969; TRN: US2201658
- Grant/Contract Number:
- SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review. B
- Additional Journal Information:
- Journal Volume: 98; Journal Issue: 21; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY
Citation Formats
Geondzhian, Andrey, and Gilmore, Keith. Demonstration of resonant inelastic x-ray scattering as a probe of exciton-phonon coupling. United States: N. p., 2018.
Web. doi:10.1103/physrevb.98.214305.
Geondzhian, Andrey, & Gilmore, Keith. Demonstration of resonant inelastic x-ray scattering as a probe of exciton-phonon coupling. United States. https://doi.org/10.1103/physrevb.98.214305
Geondzhian, Andrey, and Gilmore, Keith. Mon .
"Demonstration of resonant inelastic x-ray scattering as a probe of exciton-phonon coupling". United States. https://doi.org/10.1103/physrevb.98.214305. https://www.osti.gov/servlets/purl/1637655.
@article{osti_1637655,
title = {Demonstration of resonant inelastic x-ray scattering as a probe of exciton-phonon coupling},
author = {Geondzhian, Andrey and Gilmore, Keith},
abstractNote = {Resonant inelastic x-ray scattering (RIXS) is a promising technique for obtaining electron-phonon coupling constants. However, the ability to extract these coupling constants throughout the Brillouin zone for crystalline materials remains limited. To address this need, we developed a Green's function formalism to capture electron-phonon contributions to core-level spectroscopies without explicitly solving the full vibronic problem. Our approach is based on the cumulant expansion of the Green's function combined with many-body theory calculated vibrational coupling constants. The methodology is applied to x-ray photoemission spectroscopy, x-ray absorption spectroscopy (XAS), and RIXS. In the case of the XAS and RIXS, we use a two-particle exciton Green's function, which accounts implicitly for particle-hole interference effects that have previously proved difficult. To demonstrate the methodology and gain a deeper understanding of the experimental technique, we apply our formalism to small molecules, for which unambiguous experimental data exist. This comparison reveals that the vibronic coupling constant probed by RIXS is in fact related to exciton-phonon coupling rather than electron-phonon coupling, challenging the conventional interpretation of the experiment.},
doi = {10.1103/physrevb.98.214305},
journal = {Physical Review. B},
number = 21,
volume = 98,
place = {United States},
year = {2018},
month = {12}
}
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Figures / Tables:
FIG. 1: RIXS loss profile for two equally coupled modes. The contribution from the two mode model that includes mixing of the modes (black curve an grey shading) is compared to the independent mode approximation (red curve). In the latter case, the individual contributions from the two modes are givenmore »
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