All-Optical Valley Polarization Switch via Controlling Spin-Triplet and Spin-Singlet Interlayer Exciton Emission in WS2/WSe2 Heterostructure.

Although selective singlet and triplet interlayer exciton (IX) emission of transition metal dichalcogenides (TMD) heterostructures can be achieved by applying an electric or magnetic field, the device structure is complex and a low temperature is usually required. Here, we demonstrate a simple all-optical approach to selectively enhance the emission of singlet and triplet IX by selectively coupling singlet or triplet IX of a WS2/WSe2 heterostructure to a SiO2 microsphere cavity. Angle-resolved photoluminescene reveals that the transition dipole of triplet IX is almost along the out-of-plane direction, while singlet IX only has 69% out-of-plane dipole moment contribution. Since the out-of-plane dipole presents a higher Purcell factor within the cavity, we can simultaneously enhance the emission intensity of IX and control the emissive IX species at room temperature in an all-optical route. Importantly, we demonstrate an all-optical valley polarization switch with a record high on/off ratio of 35.

Layer-Number Engineered Momentum-Indirect Interlayer Excitons with Large Spectral Tunability.

Interlayer excitons (IXs) in type II van der Waals (vdW) heterostructures are equipped with an oriented permanent dipole moment and long lifetime and thus would allow promising applications in excitonic and optoelectronic devices. However, based on the widely studied heterostructures of transition-metal dichalcogenides (TMDs), IX emission is greatly influenced by the lattice mismatch and geometric misalignment between the constituent layers, increasing the complexity of the device fabrication. Here, we report on the robust momentum-indirect IX emission in TMD/two-dimensional (2D) perovskite vdW heterostructures, which were fabricated without considering the orientation arrangement or momentum mismatch. The IXs show a large diffusion coefficient of ∼10 cm2 s-1, and importantly the IX emission energy can be widely tuned from 1.3 to 1.6 eV via changing the layer number of the 2D perovskite or the thickness of TMD flakes, shedding light on the applications of vdW interface engineering to broad-spectrum optoelectronics.

Probing the interlayer excitation dynamics in WS2/WSe2 heterostructures with broadly tunable pump and probe energies.

van der Waals heterostructures based on transition metal dichalcogenides (TMDs) provide a fascinating platform for exploring new physical phenomena and novel optoelectronic functionalities. Revealing the energy-dependence of photocarrier population dynamics in heterostructures is key for developing optoelectronic or valleytronic devices. Here, the broadband transient dynamics of interlayer excitation of a nearly-aligned WS2/WSe2 heterostructure is investigated by using energy-dependent pump-probe spectroscopy at cryogenic temperatures. Interestingly, WS2/WSe2 interlayer excitation, herein comprising a mixture of intra- and inter-layer excitons, exhibits largely constant lifetimes of a few hundred picoseconds across a broad energy range, in stark contrast to the salient energy-dependent dynamics of intralayer excitons in monolayer WSe2. While the PL emission of the WS2/WSe2 heterostructure is found to be strongly affected by electrostatic doping, the lifetimes of interlayer excitation show negligible changes. Our work elaborates the signatures of ultrafast dynamics introduced by intra- and interlayer co-existing excitonic species and enriches the understanding of interlayer couplings in van der Waals heterostructures.