No Arabic abstract
Interlayer excitons confined in bilayer heterostructures of transition metal dichalcogenides (TMDs) offer a promising route to implement two-dimensional dipolar superfluids. Here, we study the experimental conditions necessary for the realisation of such collective state. Particularly, we show that the moire potential inherent to TMD bilayers yields an exponential increase of the excitons effective mass. To allow for exciton superfluidity at sizeable temperatures it is then necessary to intercalate a high-$kappa$ dielectric between the monolayers confining electrons and holes. Thus the moire lattice depth is sufficiently weak for a superfluid phase to theoretically emerge below a critical temperature of around 10 K. Importantly, for realistic experimental parameters interlayer excitons quasi-condense in a state with finite momentum, so that the superfluid is optically inactive and flows spontaneously.
Atomistic van der Waals heterostacks are ideal systems for high-temperature exciton condensation because of large exciton binding energies and long lifetimes. Charge transport and electron energy-loss spectroscopy showed first evidence of excitonic many-body states in such two-dimensional materials. Pure optical studies, the most obvious way to access the phase diagram of photogenerated excitons have been elusive. We observe several criticalities in photogenerated exciton ensembles hosted in MoSe2-WSe2 heterostacks with respect to photoluminescence intensity, linewidth, and temporal coherence pointing towards the transition to a coherent quantum state. For this state, the occupation is 100 percent and the exciton diffusion length is increased. The phenomena survive above 10 kelvin, consistent with the predicted critical condensation temperature. Our study provides a first phase-diagram of many-body interlayer exciton states including Bose Einstein condensation.
In van der Waals (vdW) heterostructures formed by stacking two monolayer semiconductors, lattice mismatch or rotational misalignment introduces an in-plane moire superlattice. While it is widely recognized that a moire superlattice can modulate the electronic band structure and lead to novel transport properties including unconventional superconductivity and insulating behavior driven by correlations, its influence on optical properties has not been investigated experimentally. We present spectroscopic evidence that interlayer excitons are confined by the moire potential in a high-quality MoSe2/WSe2 heterobilayer with small rotational twist. A series of interlayer exciton resonances with either positive or negative circularly polarized emission is observed in photoluminescence, consistent with multiple exciton states confined within the moire potential. The recombination dynamics and temperature dependence of these interlayer exciton resonances are consistent with this interpretation. These results demonstrate the feasibility of engineering artificial excitonic crystals using vdW heterostructures for nanophotonics and quantum information applications.
The properties of van der Waals (vdW) heterostructures are drastically altered by a tunable moire superlattice arising from periodic variations of atomic alignment between the layers. Exciton diffusion represents an important channel of energy transport in semiconducting transition metal dichalcogenides (TMDs). While early studies performed on TMD heterobilayers have suggested that carriers and excitons exhibit long diffusion lengths, a rich variety of scenarios can exist. In a moire crystal with a large supercell size and deep potential, interlayer excitons may be completely localized. As the moire period reduces at a larger twist angle, excitons can tunnel between supercells and diffuse over a longer lifetime. The diffusion length should be the longest in commensurate heterostructures where the moire superlattice is completely absent. In this study, we experimentally demonstrate that the moire potential impedes interlayer exciton diffusion by comparing a number of WSe2/MoSe2 heterostructures prepared with chemical vapor deposition and mechanical stacking with accurately controlled twist angles. Our results provide critical guidance to developing twistronic devices that explore the moire superlattice to engineer material properties.
We investigate the photoluminescence of interlayer excitons in heterostructures consisting of monolayer MoSe2 and WSe2 at low temperatures. Surprisingly, we find a doublet structure for such interlayer excitons. Both peaks exhibit long photoluminescence lifetimes of several ten nanoseconds up to 100 ns at low temperatures, which verifies the interlayer nature of both. The peak energy and linewidth of both show unusual temperature and power dependences. In particular, we observe a blue-shift of their emission energy for increasing excitation powers. At a low excitation power and low temperatures, the energetically higher peak shows several spikes. We explain the findings by two sorts of interlayer excitons; one that is indirect in real space but direct in reciprocal space, and the other one being indirect in both spaces. Our results provide fundamental insights into long-lived interlayer states in van der Waals heterostructures with possible bosonic many-body interactions
Stacking monolayers of transition metal dichalcogenides into a heterostructure with a finite twist-angle gives rise to artificial moire superlattices with a tunable periodicity. As a consequence, excitons experience a periodic potential, which can be exploited to tailor optoelectronic properties of these materials. While recent experimental studies have confirmed twist-angle dependent optical spectra, the microscopic origin of moire exciton resonances has not been fully clarified yet. Here, we combine first principle calculations with the excitonic density matrix formalism to study transitions between different moire exciton phases and their impact on optical properties of the twisted MoSe$_2$/WSe$_2$ heterostructure. At angles smaller than 2$^{circ}$ we find flat, moire trapped states for inter- and intralayer excitons. This moire exciton phase drastically changes into completely delocalized states already at 3$^{circ}$. We predict a linear and quadratic twist-angle dependence of excitonic resonances for the moire-trapped and delocalized exciton phase, respectively. Our work provides microscopic insights opening the possibility to tailor moire exciton phases in van der Waals superlattices.