Measuring momentum-resolved dissipation of phonon-polaritons in LiNbO${}_3$ with terahertz driving

Abstract

Mapping the dispersion of polaritons, hybrid quasiparticles arising from light-matter coupling, can provide key insights into the material dielectric response, coupling strength, and energy transfer pathways with other excitations. In this work, we present THz pump-Raman probe (TP-RP) as a versatile method for mapping the polariton dispersion in polar non-centrosymmetric materials, demonstrated here for the case of phonon-polaritons in LiNbO${}_3$. By resonantly driving polaritonic modes with a broadband THz pump and probing them with a tunable NIR Raman pulse, TP-RP allows for the extraction of the momentum-dependence of both their frequency and damping rate with high accuracy. The spectral features observed in the pump-probe signal, including the polaritonic response as well as pulse artifacts, are reproduced within a many-body theoretical approach. Applying the technique to study the E(TO${}_1$) phonon of LiNbO${}_3$ enables the combined analysis of theory and experiments to uncover a nontrivial frequency dependence of the phonon intrinsic damping rate, revealing possible anharmonic couplings to other modes.

29 pages, 13 figures