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Mapping LiNbO₃ Phonon-Polariton Nonlinearities with 2D THz-THz-Raman Spectroscopy

Lin, Haw-Wei and Mead, Griffin and Blake, Geoffrey A. (2022) Mapping LiNbO₃ Phonon-Polariton Nonlinearities with 2D THz-THz-Raman Spectroscopy. Physical Review Letters, 129 (20). Art. No. 207401. ISSN 0031-9007. doi:10.1103/physrevlett.129.207401.

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Two-dimensional terahertz-terahertz-Raman spectroscopy can provide insight into the anharmonicities of low-energy phonon modes—knowledge of which can help develop strategies for coherent control of material properties. Measurements on LiNbO₃ reveal THz and Raman nonlinear transitions between the E(TO₁) and E(TO₃) phonon polaritons. Distinct coherence pathways are observed with different THz polarizations. The observed pathways suggest that the origin of the third-order nonlinear responses is due to mechanical anharmonicities, as opposed to electronic anharmonicities. Further, we confirm that the E(TO₁) and E(TO₃) phonon polaritons are excited through resonant one-photon THz excitation.

Item Type:Article
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URLURL TypeDescription
Lin, Haw-Wei0000-0002-5208-7385
Mead, Griffin0000-0003-0067-4219
Blake, Geoffrey A.0000-0003-0787-1610
Additional Information:The authors acknowledge the National Science Foundation CSDM-A program (Grant No. CHE-1665467) and NASA APRA program (Grant No. 80NSSC21K1467) for financial support. H. W. L. acknowledges financial support from the Ministry of Education of Taiwan. G. M. acknowledges financial support from the National Science Foundation Graduate Research Fellowship Program.
Group:Division of Geological and Planetary Sciences
Funding AgencyGrant Number
Ministry of Education (Taipei)UNSPECIFIED
NSF Graduate Research FellowshipUNSPECIFIED
Issue or Number:20
Record Number:CaltechAUTHORS:20221205-666301600.2
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:118230
Deposited By: Research Services Depository
Deposited On:05 Jan 2023 23:41
Last Modified:05 Jan 2023 23:42

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