ArXiv · 2026
The fate of quantum coherence following photoexcitation is a central problem in nonequilibrium condensed-matter physics, especially in low-dimensional solids where electronic, structural and many-body energy scales are strongly coupled. Here, we investigate this interplay in ferroelectric α-In₂Se₃ using broadband transient-grating spectroscopy with ∼5 fs laser pulses. Photoexcitation launches pronounced oscillations dominated by a ∼104 cm⁻¹ mode that persists for several picoseconds. Measurements from 10 to 300 K show that its frequency remains nearly unchanged while its coherence is progressively suppressed, distinguishing the lattice coordinate from thermally activated dephasing. Varying excitation energy reveals a distinct crossover in which increasing photoexcitation progressively modifies and damps the coherent response. First-principles calculations assign the dominant oscillation to a 101.47 cm⁻¹ Γ-point optical phonon involving collective In-Se displacement, while quantum-dynamical simulations reproduce the main transient-grating oscillations. These results establish α-In₂Se₃ as a model system for independently probing lattice coherence, thermal fluctuations and carrier-density-dependent interactions, revealing how a polar van der Waals semiconductor evolves from coherent lattice motion toward an incoherent many-body state after ultrafast excitation.
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