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Polarization-Resolved Extreme-Ultraviolet Second-Harmonic Generation from LiNbO_{3}.

Can B Uzundal1,2, Sasawat Jamnuch3, Emma Berger1,2

  • 1Department of Chemistry, University of California, Berkeley, California 94720, USA.

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|December 22, 2021
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Extreme ultraviolet second harmonic generation (XUV-SHG) spectroscopy now offers element-resolved insights into material symmetry. This new technique distinguishes elemental contributions in LiNbO₃, revealing distortions crucial for understanding ferroelectricity.

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Area of Science:

  • Condensed Matter Physics
  • Materials Science
  • Spectroscopy

Background:

  • Second harmonic generation (SHG) spectroscopy is vital for probing surface, interfacial, and solid-state symmetry properties.
  • Current polarization-resolved SHG in visible-infrared regimes struggles with complex materials, limiting interpretation of electronic and magnetic order.
  • Investigating novel materials necessitates advanced spectroscopic methods for deeper understanding of their properties.

Purpose of the Study:

  • To demonstrate polarization-resolved extreme ultraviolet second harmonic generation (XUV-SHG) spectroscopy for the first time.
  • To enable element-resolved angular anisotropy investigations in materials.
  • To verify the applicability of dipole-based SHG models in the XUV regime.

Main Methods:

  • Development and application of polarization-resolved XUV-SHG spectroscopy.
  • Energy-dependent XUV-SHG measurements on noncentrosymmetric Lithium Niobate (LiNbO₃).
  • Computational simulations of second harmonic generation spectra based on atomic displacements.

Main Results:

  • XUV-SHG successfully distinguished elemental contributions from Lithium (Li) and Niobium (Nb) in LiNbO₃.
  • The study revealed that Li ion displacement, linked to ferroelectricity, is accompanied by NbO₆ octahedron distortions.
  • Simulations confirmed that Li ion displacement and oxygen atom movements explain the observed SHG spectrum and symmetry breaking.

Conclusions:

  • Element-resolved XUV-SHG provides unprecedented sensitivity to symmetry breaking and atomic environments.
  • The findings validate dipole-based SHG models in the XUV spectral range.
  • This work opens new avenues for time- and angle-resolved XUV-SHG studies with elemental specificity in condensed matter.