Abstract
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 LiNbO_{3} reveal THz and Raman nonlinear transitions between the E(TO_{1}) and E(TO_{3}) 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(TO_{1}) and E(TO_{3}) phonon polaritons are excited through resonant one-photon THz excitation.
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