One of the overarching goals of the entire TRR is to establish monolayer transition metal dichalcogenides (TMDCs, e.g. monolayer MoS2 or monolayer WS2) as new materials for ultrafast spintronics. The potential advantages of TMDCs for spintronics include the possibility of optical manipulation of spin/valley degrees of freedom and facile tunability of spin properties via surface modification. Recent experiments on TMDCs already confirmed coupled spin/valley carrier dynamics, strong quantum-confined excitonic effects, and long spin relaxation times. At the same time, while multiple groups probed spin dynamics in pristine TMDC materials, virtually nothing is known regarding the ultrafast evolution of spin currents at metal/TMDC interfaces. The understanding of such interfaces is crucially important for operation of any realistic device. The presence of built-in strain, built-in electric fields, and proximal magnetic fields at the TMDC/metal interface are expected to dramatically alter the spin relaxation time and affect the spin injection efficiency. The behavior of spins at the TMDC/metal interface is equally interesting from the fundamental perspective. Among predicted yet mostly unstudied phenomena are the appearance of strong strain-induced pseudomagnetic fields, proximity-induced ferromagnetism, and new excitonic phenomena. Therefore, the main goal of this project is to controllably investigate the phenomena affecting the dynamics of spins at the interface between TMDCs and metals.
Specifically, we will create model systems to study the effects of the following interfacial phenomena on the spin dynamics:
To probe these effects, we will develop time-resolved photocurrent spectroscopy (trPC), a new optoelectronic technique for probing spin transport. In trPC, the photocurrent produced in a TMDC device is measured as a function of time delay between two ultrashort light pulses exciting the sample. This optoelectronic technique is expected to allow probing devices much smaller than the diffraction limit, to be sensitive to carrier transport/diffusion, and to enable separation of the effects in TMDCs from those in proximal materials. The trPC will be complemented by time-resolved Kerr rotation microscopy (trKR). This combination of techniques allows probing the spin dynamics of excitons and free carriers in device geometries with vertical or lateral interfaces.