Observation of Negative Terahertz Photoconductivity in Large Area Type-II Dirac Semimetal PtTe2

As a newly emergent type-II Dirac semimetal, platinum telluride (PtTe2) stands out from other two dimensional noble-transition-metal dichalcogenides for the unique band structure and novel physical properties, and has been studied extensively. However, the ultrafast response of low energy quasiparticle excitation in terahertz frequency remains nearly unexplored yet. Herein, we employ optical pump-terahertz probe (OPTP) spectroscopy to systematically study the photocarrier dynamics of PtTe2 thin films with varying pump fluence, temperature, and film thickness. Upon photoexcitation the terahertz photoconductivity (PC) of PtTe2 films shows abrupt increase initially, while the terahertz PC changes into negative value in a subpicosecond timescale, followed by a prolonged recovery process that lasted a few nanoseconds. The magnitude of both positive and negative terahertz PC response shows strongly pump fluence dependence. We assign the unusual negative terahertz PC to the formation of small polaron due to the strong electron-phonon (e-ph) coupling, which is further substantiated by temperature and film thickness dependent measurements. Moreover, our investigations give a subpicosecond timescale of simultaneous carrier cooling and polaron formation. The present study provides deep insights into the underlying dynamics evolution mechanisms of photocarrier in type-II Dirac semimetal upon photoexcitation, which is of crucial importance for designing PtTe2-based optoelectronic devices.

Automated summary

In this study, the photocarrier dynamics of PtTe2 thin films were systematically studied using optical pump-terahertz probe spectroscopy. The research revealed unusual behaviors of terahertz photoconductivity and provided insights into simultaneous carrier cooling and polaron formation on a subpicosecond timescale. These findings are crucial for the design of optoelectronic devices based on PtTe2.