Comparison of coherent phonon generation by electronic and ionic Raman scattering in
Open Access
- 10 February 2021
- journal article
- research article
- Published by American Physical Society (APS) in Physical Review Research
- Vol. 3 (1), 013126
- https://doi.org/10.1103/physrevresearch.3.013126
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 . We find that the oscillatory amplitude of the low-frequency Raman-active mode exhibits a sharp peak when we tune our pump frequency into resonance with the high-frequency infrared-active 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 that alter the measured amplitude of the coherent phonon response.
Funding Information
- Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung (200021_169698, P2EZP2_184259)
- European Research Council (291151)
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