Nonlinear optical phonon spectroscopy revealing polaronic signatures of the LaAlO3/SrTiO3 interface

Sci Adv. 2023 Jun 9;9(23):eadg7037. doi: 10.1126/sciadv.adg7037. Epub 2023 Jun 9.

Abstract

We report the direct observation of lattice phonons confined at LaAlO3/SrTiO3 (LAO/STO) interfaces and STO surfaces using the sum-frequency phonon spectroscopy. This interface-specific nonlinear optical technique unveiled phonon modes localized within a few monolayers at the interface, with inherent sensitivity to the coupling between lattice and charge degrees of freedom. Spectral evolution across the insulator-to-metal transition at LAO/STO interface revealed an electronic reconstruction at the subcritical LAO thickness, as well as strong polaronic signatures upon formation of the two-dimensional electron gas. We further discovered a characteristic lattice mode from interfacial oxygen vacancies, enabling us to probe such important structural defects in situ. Our study provides a unique perspective on many-body interactions at the correlated oxide interfaces.

MeSH terms

  • Electronics*
  • Electrons
  • Oxides
  • Phonons*
  • Spectrum Analysis

Substances

  • Oxides