Thickness-dependent exciton relaxation dynamics of few-layer rhenium diselenide

Rhenium diselenide(ReSe_(2))has gathered much attention due to its low symmetry of lattice structure,which makes it possess in-plane anisotropic optical,electrical as well as excitonic properties and further enables ReSe_(2)have an important application in optoelectronic devices.Here,we report the thickness-dependent exciton relaxation dynamics of mechanically exfoliated few-layer ReSe_(2)flakes by using time-resolved pump–probe transient transmission spectroscopies.The results reveal two thickness-dependent relaxation processes of the excitons.The fast one correlates with the exciton formation(i.e.,the conversion of hot carriers to excitons),while the slow one is attributed to the exciton recombination dominated by defect-assisted exciton trapping besides photon emission channel.The decrease of scattering probability caused by defects leads to the increase of fast lifetime with thickness,and the increase of slow lifetime with thickness is related to the trap-mediated exciton depopulation induced by surface defects.Polarization-dependent transient spectroscopy indicates the isotropic exciton dynamics in the two-dimensional(2D)plane.These results are insightful for better understanding of excitonic dynamics of ReSe_(2)materials and its application in future optoelectronic and electronic devices.

Unusual photocarrier and coherent phonon dynamics behaviors of layered PdSe_(2)unveiled by ultrafast spectroscopy of the edge surface

Layered materials exhibit different electronic and phonon properties along in-plane and out-of-plane directions;existing studies focus on their in-plane behaviors,and the influence of such anisotropies on the dynamics of photocarriers and phonons is unknown.Here,we fabricate layered PdSe_(2)crystals with flat edge surfaces and compare the time-resolved ultrafast spectroscopies on their basal and edge surfaces.Pronounced differences in the transient reflection spectroscopies reveal the inconsistent photocarrier and phonon dynamics behaviors on the two surfaces:the slow hot carrier relaxation process is accelerated and the thermoelasticity-induced longitudinal coherent acoustic phonon oscillation completely vanishes on the edge surface,as compared with the basal surface.Theoretical analysis reveals that the inconsistent hot carrier dynamics originate from the anisotropic properties of low-energy phonons in PdSe_(2),and the absence of phonon oscillation on the edge surface results from the wavevector-limited sensitivity of acoustic B_(1u)mode.Moreover,polarization-dependent spectroscopies indicate the diverse optical anisotropies beyond the in-plane of PdSe_(2).This work provides a new method to explore unique physical properties and modulate the optical anisotropy of layered materials.