Collective interlayer pairing and pair superfluidity in vertically stacked layers of dipolar excitons

Layered bosonic dipolar fluids have been suggested to host a condensate of interlayer molecular bound states. However, experimental observation has remained elusive. Motivated by two recent experimental works [C. Hubert et al., Phys. Rev. X9, 021026 (2019) and D. J. Choksy et al., Phys. Rev. B 103, 045126 (2021)], we theoretically study, using numerically exact quantum Monte Carlo calculations, the experimental signatures of collective interlayer pairing in vertically stacked indirect exciton (IX) layers. We find that IX energy shifts associated with each layer evolve nontrivially as a function of density imbalance following a nonmonotonic trend with a jump discontinuity at density balance, identified with the interlayer IX molecule gap. This behavior discriminates between the superfluidity of interlayer bound pairs and independent dipole condensation in distinct layers. Considering finite temperature and finite density imbalance conditions, we find a cascade of Berezinskii-Kosterlitz-Thouless (BKT) transitions, initially into a pair superfluid and only then, at lower temperatures, into complete superfluidity of both layers. Our results may provide a theoretical interpretation of existing experimental observations in GaAs double quantum well (DQW) bilayer structures. Furthermore, to optimize the visibility of pairing dynamics in future studies, we present an analysis suggesting realistic experimental settings in GaAs and transition metal dichalcogenide (TMD) bilayer DQW heterostructures where collective interlayer pairing and pair superfluidity can be clearly observed.