Long-lived relaxation channel and exciton-phonon coupling in Ta2NiSe5 via non-degenerate pump-probe spectroscopy

Abstract

An excitonic insulator represents a quantum phase in which spontaneous condensation of excitons leads to novel many-body phenomena. Ta${}_2$NSi${}_5$ (TNSe), a layered narrow-gap semiconductor, has emerged as a model platform to probe these correlated excitonic phases and their underlying dynamics below 327 K. In this work, we investigate the nonequilibrium dynamics of TNSe using temperature-dependent, non-degenerate optical pump-probe spectroscopy with a 3.14 eV pump and a 1.57 eV probe, extending the accessible pump-probe delay window up to 500 ps. In addition to the well-established sub-picosecond relaxation channel ($\sim$ 0.7- 0.9 ps) associated with carrier cooling and recombination, accompanied by exciton reformation, we uncover a much slower recovery process with a decay time of $\sim$ 280-600~ps, significantly longer than previously reported. We attribute this unusually prolonged recovery to enhanced scattering between excitons and nonequilibrium phonons, which delays the re-establishment of equilibrium excitonic correlations. On top of this bi-exponential background, we observe two coherent phonon modes at 1.0 and 2.9 THz with distinctly different coupling behaviors. The 1.0 THz mode exhibits an order-parameter-like temperature dependence, consistent with strong coupling to the excitonic condensate in TNSe. In contrast, the 2.9 THz mode does not exhibit any discernible coupling to the excitonic order parameter, and appears to arise from anharmonic lattice dynamics associated with the structural phase transition. Together, these results elucidate the hierarchy of relaxation pathways in TNSe and highlight the importance of extending the temporal detection window in pump-probe measurements to fully capture long-lived exciton-phonon dynamics.

5 Main figures, 9 supplemental figures

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