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Current vs Charge Density Contributions to Nonlinear X-ray Spectroscopy.

Jérémy R Rouxel1, Markus Kowalewski1, Shaul Mukamel1

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Summary

This study introduces a nonlocal response tensor to analyze nonlinear X-ray signals, linking them to current and charge densities. It clarifies the roles of different coupling terms in resonant and off-resonant scattering processes.

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Area of Science:

  • Nonlinear optics
  • X-ray physics
  • Quantum electrodynamics

Background:

  • Nonlinear X-ray signals are crucial for probing matter.
  • Current descriptions often rely on multipole expansions.
  • A deeper understanding of scattering mechanisms is needed.

Purpose of the Study:

  • To express stimulated and spontaneous nonlinear X-ray signals using a nonlocal response tensor.
  • To connect these signals directly to time-evolving current and charge densities.
  • To elucidate the relative contributions of different coupling terms in X-ray scattering.

Main Methods:

  • Formulation of a spatially nonlocal response tensor.
  • Analysis of stimulated (coherent) and spontaneous (incoherent) nonlinear X-ray signals.
  • Investigation of minimal coupling terms (σA(2) and j · A).

Main Results:

  • The nonlocal response tensor directly links X-ray signals to current (j) and charge (σ) densities.
  • The σA(2) term dominates off-resonant scattering.
  • The j · A term dominates resonant scattering.
  • Both terms contribute comparably near resonant detunings.

Conclusions:

  • The nonlocal response tensor provides a more direct link to fundamental charge and current dynamics.
  • This framework clarifies the distinct roles of coupling terms in different scattering regimes.
  • The findings offer a refined understanding of nonlinear X-ray interactions.