Photoexcited carrier dynamics and magnetic order-induced band splittings in CrSiTe₃

Magnetic van der Waals 2D ferromagnetic semiconductors hold great promise for future spin-optoelectronic. Understanding how materials properties are impacted by magnetic ordering and the spin-orbit interactions is critically needed information for the development of applications. We use ultrafast transient reflectance (TR) and photocurrent (PC) spectroscopies to investigate the band structure and photoexcited carrier dynamics of a CrSiTe₃ (CST) nanosheet in the paramagnetic (PM, 300K) and ferromagnetic (FM, 10 K) phases. We observe both a decrease of the direct bandgap and emergence of a 120 meV splitting of the direct optical transition when the FM phase is present. DFT band structure calculations which include spin-orbit coupling suggest that the band modifications are driven by a FM ordering-induced band splitting between the Te ?? and the Cr ?? states at the valence and conduction band edges. We find that the majority of carriers photoexcited at the direct gap recombine within picoseconds through defect-mediated recombination, but that 2-3 % of the electrons scatter into indirect conduction band valleys resulting in very long-lived electrons and holes. Those long-lived carriers contribute to the broadband PC response of CST devices that also features indirect absorption. These results provide critical insights into the dynamics and energy landscape of photoexcited electrons and holes, and how they are impacted by spin-ordering effects in layered ferromagnets.