Demonstration of resonant inelastic x-ray scattering as a probe of exciton-phonon coupling

Geondzhian, Andrey; Gilmore, Keith

doi:10.1103/physrevb.98.214305

Title: Demonstration of resonant inelastic x-ray scattering as a probe of exciton-phonon coupling

Journal Article · 10 December 2018 · Physical Review. B

DOI: https://doi.org/10.1103/physrevb.98.214305 · OSTI ID:1637655

Geondzhian, Andrey ^[1];

^[1]

Brookhaven National Lab. (BNL), Upton, NY (United States)

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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 1637655

Report Number(s):: BNL-216122-2020-JAAM; 2469-9969; TRN: US2201658

Journal Information:: Physical Review. B, Vol. 98, Issue 21; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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