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Title: Multiple core-hole coherence in x-ray four-wave-mixing spectroscopies

Abstract

Correlation-function expressions are derived for the coherent nonlinear response of molecules to three resonant ultrafast pulses in the x-ray regime. The ability to create two-core-hole states with controlled attosecond timing in four-wave-mixing and pump probe techniques should open up new windows into the response of valence electrons, which are not available from incoherent x-ray Raman and fluorescence spectroscopy. Closed expressions for the necessary four-point correlation functions are derived for the electron-boson model by using the second order cumulant expansion to describe the fluctuating potentials. The information obtained from multidimensional nonlinear techniques could be used to test and refine this model, and establish an anharmonic oscillator picture for electronic excitations.

Authors:
 [1]
  1. Department of Chemistry, University of California, Irvine, Irvine, California 92697-2025 (United States)
Publication Date:
OSTI Identifier:
20787770
Resource Type:
Journal Article
Resource Relation:
Journal Name: Physical Review. B, Condensed Matter and Materials Physics; Journal Volume: 72; Journal Issue: 23; Other Information: DOI: 10.1103/PhysRevB.72.235110; (c) 2005 The American Physical Society; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; ANHARMONIC OSCILLATORS; BOSONS; CORRELATION FUNCTIONS; ELECTRON CORRELATION; ELECTRONS; EXCITATION; EXCITED STATES; FLUORESCENCE SPECTROSCOPY; FREQUENCY MIXING; HARMONIC OSCILLATORS; HOLES; MOLECULES; NONLINEAR PROBLEMS; OPTICAL PUMPING; POTENTIALS; PULSES; VALENCE; VELOCITY; X RADIATION

Citation Formats

Mukamel, Shaul. Multiple core-hole coherence in x-ray four-wave-mixing spectroscopies. United States: N. p., 2005. Web. doi:10.1103/PHYSREVB.72.2.
Mukamel, Shaul. Multiple core-hole coherence in x-ray four-wave-mixing spectroscopies. United States. doi:10.1103/PHYSREVB.72.2.
Mukamel, Shaul. Thu . "Multiple core-hole coherence in x-ray four-wave-mixing spectroscopies". United States. doi:10.1103/PHYSREVB.72.2.
@article{osti_20787770,
title = {Multiple core-hole coherence in x-ray four-wave-mixing spectroscopies},
author = {Mukamel, Shaul},
abstractNote = {Correlation-function expressions are derived for the coherent nonlinear response of molecules to three resonant ultrafast pulses in the x-ray regime. The ability to create two-core-hole states with controlled attosecond timing in four-wave-mixing and pump probe techniques should open up new windows into the response of valence electrons, which are not available from incoherent x-ray Raman and fluorescence spectroscopy. Closed expressions for the necessary four-point correlation functions are derived for the electron-boson model by using the second order cumulant expansion to describe the fluctuating potentials. The information obtained from multidimensional nonlinear techniques could be used to test and refine this model, and establish an anharmonic oscillator picture for electronic excitations.},
doi = {10.1103/PHYSREVB.72.2},
journal = {Physical Review. B, Condensed Matter and Materials Physics},
number = 23,
volume = 72,
place = {United States},
year = {Thu Dec 15 00:00:00 EST 2005},
month = {Thu Dec 15 00:00:00 EST 2005}
}