Probing strong electron-phonon coupling in semimetallic PtSe2 via ultrafast optical spectroscopy
摘要
Platinum diselenide (PtSe2) exhibits a distinctive thickness-modulated metal-to-semiconductor transition, which makes it suitable for diverse applications in nanoelectronics and optoelectronics. This study systematically investigates the spatiotemporal dynamics of photoexcited carrier relaxation in PtSe2. Through temperature-dependent ultrafast spectroscopy, two distinct low-frequency acoustic phonons (AP) were identified in multilayer PtSe2. Transient absorption microscopy (TAM) measurements reveal thickness-dependent relaxation dynamics and distinct carrier diffusion behavior in multilayer PtSe2. These findings indicate superior carrier transport properties, with a measured mobility of 394.1±38.5 cm2·V−1·s−1 for multilayers. Temperature-dependent ultrafast dynamics, acquired using a custom-built cryogenic pump-probe system, reveal two coherent AP modes, ω1 and ω2, with central frequencies of 1.27 and 0.17 THz, respectively. The higher frequency ω1 mode corresponds to shear mode with a nominal electron-phonon coupling constant λω1 = 2.22. To our knowledge, this study represents a pioneering investigation that employs low-temperature ultrafast spectroscopy to elucidate the AP mode and strong electron-phonon coupling in semimetallic PtSe2 systems. These findings offer fundamental insights into the semimetallic nature of PtSe2 and establish a basis for designing ultrafast photonic devices that harness its distinct optoelectronic response.