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Published in

American Association for the Advancement of Science, Science Advances, 23(9), 2023

DOI: 10.1126/sciadv.adg7037

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Nonlinear optical phonon spectroscopy revealing polaronic signatures of the LaAlO <sub>3</sub> /SrTiO <sub>3</sub> interface

This paper is made freely available by the publisher.
This paper is made freely available by the publisher.

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Abstract

We report the direct observation of lattice phonons confined at LaAlO 3 /SrTiO 3 (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.