DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

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

Journal Article · · Physical Review. B

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.

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

References (83)

Photoemission Study of a Strongly Coupled Electron-Phonon System journal July 1999
Raman spectroscopy of graphene and graphite: Disorder, electron–phonon coupling, doping and nonadiabatic effects journal July 2007
Electron-Phonon Renormalization of the Direct Band Gap of Diamond journal December 2010
Effective Tunneling Density of States in Superconductors journal April 1963
Electron-Phonon Interaction in N-Doped Cuprates: an Inelastic X-Ray Scattering Study journal March 2003
Physical Origin of Satellites in Photoemission of Doped Graphene: An Ab Initio G W Plus Cumulant Study journal April 2013
Ab Initio Calculation of Excitonic Effects in the Optical Spectra of Semiconductors journal May 1998
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials journal September 2009
Raman-scattering study of exciton-phonon coupling in PbS nanocrystals journal April 1997
Determining the electron-phonon coupling strength from Resonant Inelastic X-ray Scattering at transition metal L-edges journal July 2011
Über die Streuung von Strahlung durch Atome journal February 1925
Resonant inelastic x-ray scattering studies of elementary excitations journal June 2011
Band Structures of Plasmonic Polarons journal April 2015
Dynamical properties of X-ray Raman scattering journal January 2003
Ab Initio Finite-Temperature Excitons journal September 2008
X-Ray Absorption Spectra of Water from First Principles Calculations journal May 2006
One-phonon resonant Raman scattering: Fröhlich exciton-phonon interaction journal August 1989
Particle-hole cumulant approach for inelastic losses in x-ray spectra journal July 2016
Dynamic Jahn-Teller Effect and Colossal Magnetoresistance in La 1 − x Sr x MnO 3 journal July 1996
Toward a comprehensive understanding of solid-state core-level XPS linewidths: Experimental and theoretical studies on the Si   2 p and O   1 s linewidths in silicates journal August 2009
On the use of Raman scattering to probe exciton–phonon coupling in molecular crystals journal February 1975
Many-body correlations and excitonic effects in semiconductor spectroscopy journal January 2006
Multiple Plasmon Satellites in Na and Al Spectral Functions from Ab Initio Cumulant Expansion journal September 1996
Electronic excitations: density-functional versus many-body Green’s-function approaches journal June 2002
Real-time cumulant approach for charge-transfer satellites in x-ray photoemission spectra journal March 2015
Spin-Hall Conductivity in Electron-Phonon Coupled Systems journal August 2006
Influence of core hole screening on molecular Auger rates and inner-shell lifetimes journal March 1994
Selective gating to vibrational modes through resonant X-ray scattering journal January 2017
Directly Characterizing the Relative Strength and Momentum Dependence of Electron-Phonon Coupling Using Resonant Inelastic X-Ray Scattering journal October 2016
Inelastic X-ray scattering in YBa2Cu3O6.6 reveals giant phonon anomalies and elastic central peak due to charge-density-wave formation journal November 2013
Revisiting the origin of satellites in core-level photoemission of transparent conducting oxides: The case of n -doped SnO 2 journal April 2018
Electron-lattice interactions strongly renormalize the charge-transfer energy in the spin-chain cuprate Li2CuO2 journal February 2016
Threshold singularities of the x-ray Raman scattering in metals journal October 1974
Exciton–Phonon Interactions in Molecular Crystals journal February 1970
Electron-phonon interactions from first principles journal February 2017
Intramolecular soft modes and intermolecular interactions in liquid acetone journal October 2011
Photoemission and inverse-photoemission study of superconducting YNi 2 B 2 C: Effects of electron-electron and electron-phonon interactions journal October 1994
Ab Initio Approach to Second-order Resonant Raman Scattering Including Exciton-Phonon Interaction journal August 2017
Vibrational effects on SrTiO 3 Ti 1s absorption spectra studied using first-principles methods journal August 2008
A Relativistic Equation for Bound-State Problems journal December 1951
Bethe-Salpeter equation calculations of core excitation spectra journal March 2011
Efficient implementation of core-excitation Bethe–Salpeter equation calculations journal December 2015
Comments on exciton phonon coupling: Temperature dependence journal August 1976
Observation of phonons with resonant inelastic x-ray scattering journal November 2010
Role of Lattice Coupling in Establishing Electronic and Magnetic Properties in Quasi-One-Dimensional Cuprates journal June 2013
Hybridization and electron-phonon coupling in ferroelectric BaTiO 3 probed by resonant inelastic x-ray scattering journal November 2016
Singularities in the X-Ray Spectra of Metals journal January 1970
Corrections to Migdal’s theorem for spectral functions: A cumulant treatment of the time-dependent Green’s function journal October 1994
Ab initio G W plus cumulant calculation for isolated band systems: Application to organic conductor ( TMTSF ) 2 PF 6 and transition-metal oxide SrVO 3 journal February 2016
Dynamical effects in electron spectroscopy journal November 2015
Anomalous Natural Linewidth in the 2 p Photoelectron Spectrum of S i F 4 journal November 2002
Theoretical simulations of oxygen K -edge resonant inelastic x-ray scattering of kaolinite journal April 2017
Effect of Exciton-Phonon Coupling in the Calculated Optical Absorption of Carbon Nanotubes journal January 2005
Vibrationally resolved O 1s photoelectron spectrum of water journal October 2003
Optical absorption spectra of the Holstein molecular crystal for weak and intermediate electronic coupling journal July 2002
The GW plus cumulant method and plasmonic polarons: application to the homogeneous electron gas* journal November 2016
Direct observation of the electron-phonon coupling between empty states in graphite via high-resolution electron energy-loss spectroscopy journal April 2017
Electron–vibration coupling induced renormalization in the photoemission spectrum of diamondoids journal April 2016
Theory of Superconductivity journal December 1957
Cumulant expansion for phonon contributions to the electron spectral function journal November 2014
Electron-Phonon Coupling in the Bulk of Anatase TiO 2 Measured by Resonant Inelastic X-Ray Spectroscopy journal August 2015
Electron-phonon coupling effects explored by inelastic neutron scattering journal January 2005
Phonon spectra in pure and carbon doped MgB2 by inelastic X-ray scattering journal June 2007
Ground state potential energy surfaces around selected atoms from resonant inelastic x-ray scattering journal January 2016
A new formula to calculate Franck–Condon factors for displaced and distorted harmonic oscillators journal July 2005
Excitonic Effects and the Optical Absorption Spectrum of Hydrogenated Si Clusters journal April 1998
Many-Particle Physics book January 1990
Singularities in the X-Ray Absorption and Emission of Metals. III. One-Body Theory Exact Solution journal February 1969
Electron–Phonon Interactions in an Insulator journal February 1975
Valence Electron Photoemission Spectrum of Semiconductors: Ab Initio Description of Multiple Satellites journal October 2011
Electron-Hole Excitations in Semiconductors and Insulators journal September 1998
Evidence for ubiquitous strong electron–phonon coupling in high-temperature superconductors journal August 2001
Cumulant expansion of the retarded one-electron Green function journal August 2014
Ab Initio Inclusion of Electron-Hole Attraction: Application to X-Ray Absorption and Resonant Inelastic X-Ray Scattering journal January 1998
Ubiquitous strong electron–phonon coupling at the interface of FeSe/SrTiO3 journal February 2017
Raman Scattering, Luminescence, and Exciton-Phonon Coupling in Cu 2 O journal December 1972
Thermal conductivity and phonon transport properties of silicon using perturbation theory and the environment-dependent interatomic potential journal September 2009
Dynamical screening in correlated metals: Spectral properties of SrVO 3 in the G W approximation and beyond journal April 2013
Effects of Recoil on Shake-Up Spectra in Metals journal January 1980
Numerical quantification of the vibronic broadening of the SrTiO 3 Ti L-edge spectrum journal July 2010
Scanning tunneling spectroscopy of high-temperature superconductors journal March 2007
Quasiparticles and phonon satellites in spectral functions of semiconductors and insulators: Cumulants applied to the full first-principles theory and the Fröhlich polaron journal March 2018
First-principles calculations of x-ray absorption in a scheme based on ultrasoft pseudopotentials: From α -quartz to high- T c compounds journal August 2009

Cited By (1)


Figures / Tables (9)