Electrically Tunable Valley Dynamics in Twisted WSe₂/WSe₂ Bilayers

The twist degree of freedom provides a powerful new tool for engineering the electrical and optical properties of van der Waals heterostructures. Here, we show that the twist angle can be used to control the spin-valley properties of transition metal dichalcogenide bilayers by changing the momentum alignment of the valleys in the two layers. Specifically, we observe that the interlayer excitons in twisted WSe₂/WSe₂ bilayers exhibit a high (>60%) degree of circular polarization (DOCP) and long valley lifetimes (>40  ns) at zero electric and magnetic fields. The valley lifetime can be tuned by more than 3 orders of magnitude via electrostatic doping, enabling switching of the DOCP from ∼80% in the n-doped regime to <5% in the p-doped regime. These results open up new avenues for tunable chiral light-matter interactions, enabling novel device schemes that exploit the valley degree of freedom

Electrically Tunable Valley Dynamics in Twisted WSe₂/WSe₂ Bilayers

The twist degree of freedom provides a powerful new tool for engineering the electrical and optical properties of van der Waals heterostructures. Here, we show that the twist angle can be used to control the spin-valley properties of transition metal dichalcogenide bilayers by changing the momentum alignment of the valleys in the two layers. Specifically, we observe that the interlayer excitons in twisted WSe₂/WSe₂ bilayers exhibit a high (>60%) degree of circular polarization (DOCP) and long valley lifetimes (>40  ns) at zero electric and magnetic fields. The valley lifetime can be tuned by more than 3 orders of magnitude via electrostatic doping, enabling switching of the DOCP from ∼80% in the n-doped regime to <5% in the p-doped regime. These results open up new avenues for tunable chiral light-matter interactions, enabling novel device schemes that exploit the valley degree of freedom

Excitons in a reconstructed moiré potential in twisted WSe₂/WSe₂ homobilayers

Moiré superlattices in twisted van der Waals materials have recently emerged as a promising platform for engineering electronic and optical properties. A major obstacle to fully understanding these systems and harnessing their potential is the limited ability to correlate direct imaging of the moiré structure with optical and electronic properties. Here we develop a secondary electron microscope technique to directly image stacking domains in fully functional van der Waals heterostructure devices. After demonstrating the imaging of AB/BA and ABA/ABC domains in multilayer graphene, we employ this technique to investigate reconstructed moiré patterns in twisted WSe₂/WSe₂ bilayers and directly correlate the increasing moiré periodicity with the emergence of two distinct exciton species in photoluminescence measurements. These states can be tuned individually through electrostatic gating and feature different valley coherence properties. We attribute our observations to the formation of an array of two intralayer exciton species that reside in alternating locations in the superlattice, and open up new avenues to realize tunable exciton arrays in twisted van der Waals heterostructures, with applications in quantum optoelectronics and explorations of novel many-body systems

Broken mirror symmetry in excitonic response of reconstructed domains in twisted MoSe₂/MoSe₂ bilayers

Van der Waals heterostructures obtained via stacking and twisting have been used to create moiré superlattices, enabling new optical and electronic properties in solid-state systems. Moiré lattices in twisted bilayers of transition metal dichalcogenides (TMDs) result in exciton trapping, host Mott insulating and superconducting states6 and act as unique Hubbard systems whose correlated electronic states can be detected and manipulated optically. Structurally, these twisted heterostructures feature atomic reconstruction and domain formation. However, due to the nanoscale size of moiré domains, the effects of atomic reconstruction on the electronic and excitonic properties have not been systematically investigated. Here we use near-0°-twist-angle MoSe₂/MoSe₂ bilayers with large rhombohedral AB/BA domains to directly probe the excitonic properties of individual domains with far-field optics. We show that this system features broken mirror/inversion symmetry, with the AB and BA domains supporting interlayer excitons with out-of-plane electric dipole moments in opposite directions. The dipole orientation of ground-state Γ–K interlayer excitons can be flipped with electric fields, while higher-energy K–K interlayer excitons undergo field-asymmetric hybridization with intralayer K–K excitons. Our study reveals the impact of crystal symmetry on TMD excitons and points to new avenues for realizing topologically non-trivial systems, exotic metasurfaces, collective excitonic phases and quantum emitter arrays via domain-pattern engineering