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Title: Theory of time-resolved Raman scattering in correlated systems: Ultrafast engineering of spin dynamics and detection of thermalization

Abstract

Ultrafast characterization and control of many-body interactions and elementary excitations are critical to understanding and manipulating emergent phenomena in strongly correlated systems. In particular, spin interaction plays an important role in unconventional superconductivity, but efficient tools for probing spin dynamics, especially out of equilibrium, are still lacking. To address this question, we develop a theory for nonresonant time-resolved Raman scattering, which can be a generic and powerful tool for nonequilibrium studies. We also use exact diagonalization to simulate the pump-probe dynamics of correlated electrons in the square-lattice single-band Hubbard model. Different ultrafast processes are shown to exist in the time-resolved Raman spectra and dominate under different pump conditions. For high-frequency and off-resonance pumps, we show that the Floquet theory works well in capturing the softening of bimagnon excitation. By comparing the Stokes and anti-Stokes spectra, we also show that effective heating dominates at small pump fluences, while a coherent many-body effect starts to take over at larger pump amplitudes and frequencies on resonance to the Mott gap. In conclusion, time-resolved Raman scattering thereby provides the platform to explore different ultrafast processes and design material properties out of equilibrium.

Authors:
 [1];  [2];  [3]
  1. Harvard Univ., Cambridge, MA (United States)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)
  3. Univ. of Alabama at Birmingham, Birmingham, AL (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1490060
Alternate Identifier(s):
OSTI ID: 1484416
Grant/Contract Number:  
FA9550-14-1-0035; AC02-76SF00515; AC02-05CH11231; OIA-1738698
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 98; Journal Issue: 24; 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

Wang, Yao, Devereaux, Thomas P., and Chen, Cheng -Chien. Theory of time-resolved Raman scattering in correlated systems: Ultrafast engineering of spin dynamics and detection of thermalization. United States: N. p., 2018. Web. doi:10.1103/physrevb.98.245106.
Wang, Yao, Devereaux, Thomas P., & Chen, Cheng -Chien. Theory of time-resolved Raman scattering in correlated systems: Ultrafast engineering of spin dynamics and detection of thermalization. United States. doi:10.1103/physrevb.98.245106.
Wang, Yao, Devereaux, Thomas P., and Chen, Cheng -Chien. Tue . "Theory of time-resolved Raman scattering in correlated systems: Ultrafast engineering of spin dynamics and detection of thermalization". United States. doi:10.1103/physrevb.98.245106. https://www.osti.gov/servlets/purl/1490060.
@article{osti_1490060,
title = {Theory of time-resolved Raman scattering in correlated systems: Ultrafast engineering of spin dynamics and detection of thermalization},
author = {Wang, Yao and Devereaux, Thomas P. and Chen, Cheng -Chien},
abstractNote = {Ultrafast characterization and control of many-body interactions and elementary excitations are critical to understanding and manipulating emergent phenomena in strongly correlated systems. In particular, spin interaction plays an important role in unconventional superconductivity, but efficient tools for probing spin dynamics, especially out of equilibrium, are still lacking. To address this question, we develop a theory for nonresonant time-resolved Raman scattering, which can be a generic and powerful tool for nonequilibrium studies. We also use exact diagonalization to simulate the pump-probe dynamics of correlated electrons in the square-lattice single-band Hubbard model. Different ultrafast processes are shown to exist in the time-resolved Raman spectra and dominate under different pump conditions. For high-frequency and off-resonance pumps, we show that the Floquet theory works well in capturing the softening of bimagnon excitation. By comparing the Stokes and anti-Stokes spectra, we also show that effective heating dominates at small pump fluences, while a coherent many-body effect starts to take over at larger pump amplitudes and frequencies on resonance to the Mott gap. In conclusion, time-resolved Raman scattering thereby provides the platform to explore different ultrafast processes and design material properties out of equilibrium.},
doi = {10.1103/physrevb.98.245106},
journal = {Physical Review B},
number = 24,
volume = 98,
place = {United States},
year = {2018},
month = {12}
}

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