Comparison of coherent phonon generation by electronic and ionic Raman scattering in LaAlO3


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Date

2021-02

Publication Type

Journal Article

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yes

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Abstract

In ionic Raman scattering, infrared-active phonons mediate a scattering process that results in the creation or destruction of a Raman-active phonon. This mechanism relies on nonlinear interactions between phonons and has in recent years been associated with a variety of emergent lattice-driven phenomena in complex transition-metal oxides, but the underlying mechanism is often obscured by the presence of multiple coupled order parameters in play. Here, we use time-resolved spectroscopy to compare coherent phonons generated by ionic Raman scattering with those created by more conventional electronic Raman scattering on the nonmagnetic and non-strongly-correlated wide-band-gap insulator LaAlO3. We find that the oscillatory amplitude of the low-frequency Raman-active Eg mode exhibits a sharp peak when we tune our pump frequency into resonance with the high-frequency infrared-active Eu mode, consistent with first-principles calculations. Our results suggest that ionic Raman scattering can strongly dominate electronic Raman scattering in wide-band-gap insulating materials. We also see evidence of competing scattering channels at fluences above 28mJ/cm2 that alter the measured amplitude of the coherent phonon response.

Publication status

published

Editor

Book title

Volume

3 (1)

Pages / Article No.

13126

Publisher

American Physical Society

Event

Edition / version

Methods

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Date collected

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Subject

Anharmonic lattice dynamics; Electron-phonon coupling; Optical phonons; perovskite; wide band gap systems; Femtosecond laser spectroscopy; Time-resolved light scattering spectroscopy

Organisational unit

03903 - Spaldin, Nicola A. / Spaldin, Nicola A. check_circle
03920 - Johnson, Steven / Johnson, Steven check_circle

Notes

Funding

169698 - Nonlinear phononic control over transition metal perovskites and interfaces (SNF)
291151 - Coupled and Competing Instabilities in Complex Oxides (EC)

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