Comprehensive excited state carrier dynamics of 2D selenium: One-photon and multi-photon absorption regimes

Semiconductors play a critical role in optoelectronic applications, and recent research has identified group-VI 2D semiconductors as promising materials for this purpose. Here, we report the comprehensive excited state carrier dynamics of bilayer, two-dimensional (2D) selenium (Se) in one-photon and multi-photon absorption regimes using transient reflection (TR) spectroscopy. Carrier lifetime obtained from TR measurement is used to theoretically predict the photo-responsivity for 2D Se photo-detectors operating in the one-photon-absorption regime. We also calculate a giant two-photon absorption cross section of 2.9×105 GM at 750 nm hinting possible application of 2D Se as a sub-bandgap photo-detector. The carrier recombination process is dominated by surface and sub-surface defect states in one- and multi-photon absorption regimes, respectively, resulting nearly one order increased carrier lifetime in a three-photon-absorption regime (1700 ps) compared to a one-photon-absorption regime (103 ps). Femtosecond Z-scan measurement shows saturation behavior for above bandgap excitation, further indicating the possibility of 2D Se as a saturable absorber material for passive Q-switching. Our study provides comprehensive insight into the excited state carrier dynamics of bilayer 2D Se and highlights its potential as a versatile material for various linear and non-linear optoelectronic applications.