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Coupling degrees of freedom of distinct nature plays a critical role innumerous physical phenomena. The recent emergence of layered materials providesa laboratory for studying the interplay between internal quantum degrees offreedom of electrons. Here, we report experimental signatures of new couplingphenomena connecting real spin with layer pseudospins in bilayer WSe2. Inpolarization-resolved photoluminescence measurements, we observe large spinorientation of neutral and charged excitons generated by both circularly andlinearly polarized light, with a splitting of the trion spectrum into a doubletat large vertical electrical field. These observations can be explained bylocking of spin and layer pseudospin in a given valley. Because up and downspin states are localized in opposite layers, spin relaxation is substantiallysuppressed, while the doublet emerges as a manifestation of electricallyinduced spin splitting resulting from the interlayer bias. The observeddistinctive behavior of the trion doublet under circularly and linearlypolarized light excitation further provides spectroscopic evidence ofinterlayer and intralayer trion species, a promising step toward opticalmanipulation in van der Waals heterostructures through the control ofinterlayer excitons.

Spin-Layer Locking Effects in Optical Orientation of Exciton Spin in Bilayer WSe2