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Two-dimensional semiconductors feature valleytronics phenomena due to lockingof the spin and momentum valley of the electrons. However, the valleypolarization is intrinsically limited in monolayer crystals by the fastintervalley electron-hole exchange. Hetero-bilayer crystals have been shown tohave a longer exciton lifetime and valley depolarization time. But the reportedvalley polarization was low; the valley selection rules and mechanisms ofvalley depolarization remains controversial. Here, we report singlet andbrightened triplet interlayer excitons both with over 80% valley polarizations,cross- and co-polarized with the pump laser, respectively. This is achieved inWSe2/MoSe2 hetero-bilayers with precise momentum valley alignment and narrowemission linewidth. The high valley polarizations allow us to identify the bandminima in a hetero-structure and con_rm unambiguously the direct band-gapexciton transition, ultrafast charge separation, strongly suppressed valleydepolarization. Our results pave the way for using semiconductor heterobilayersto control valley selection rules for valleytronic applications.

Highly Valley-Polarized Singlet and Triplet Interlayer Excitons in van der Waals Heterostructure