Moiré superlattices in twisted two-dimensional halide perovskites.

Moiré superlattices have emerged as a new platform for studying strongly correlated quantum phenomena, but these systems have been largely limited to van der Waals layer two-dimensional materials. Here we introduce moiré superlattices leveraging ultrathin, ligand-free halide perovskites, facilitated by ionic interactions. Square moiré superlattices with varying periodic lengths are clearly visualized through high-resolution transmission electron microscopy. Twist-angle-dependent transient photoluminescence microscopy and electrical characterizations indicate the emergence of localized bright excitons and trapped charge carriers near a twist angle of ~10°. The localized excitons are accompanied by enhanced exciton emission, attributed to an increased oscillator strength by a theoretically predicted flat band. This research showcases the promise of two-dimensional perovskites as unique room-temperature moiré materials.

Interlayer exciton landscape in WS2/tetracene heterostructures.

The vertical stacking of two-dimensional materials into heterostructures gives rise to a plethora of intriguing optoelectronic properties and presents an unprecedented potential for technological development. While much progress has been made combining different monolayers of transition metal dichalcogenides (TMDs), little is known about TMD-based heterostructures including organic layers of molecules. Here, we present a joint theory-experiment study on a TMD/tetracene heterostructure demonstrating clear signatures of spatially separated interlayer excitons in low temperature photoluminescence spectra. Here, the Coulomb-bound electrons and holes are localized either in the TMD or in the molecule layer, respectively. We reveal both in theory and experiment signatures of the entire intra- and interlayer exciton landscape in the photoluminescence spectra. In particular, we find both in theory and experiment a pronounced transfer of intensity from the intralayer TMD exciton to a series of energetically lower interlayer excitons with decreasing temperature. In addition, we find signatures of phonon-sidebands stemming from these interlayer exciton states. Our findings shed light on the microscopic nature of interlayer excitons in TMD/molecule heterostructures and could have important implications for technological applications of these materials.

Enhanced excitonic features in an anisotropic ReS2/WSe2 heterostructure.

Two-dimensional (2D) semiconductors have opened new horizons for future optoelectronic applications through efficient light-matter and many-body interactions at quantum level. Anisotropic 2D materials like rhenium disulphide (ReS2) present a new class of materials with polarized excitonic resonances. Here, we demonstrate a WSe2/ReS2 heterostructure which exhibits a significant photoluminescence quenching at room temperature as well as at low temperatures. This indicates an efficient charge transfer due to the electron-hole exchange interaction. The band alignment of two materials suggests that electrons optically injected into WSe2 are transferred to ReS2. Polarization resolved luminescence measurements reveal two additional polarization-sensitive exciton peaks in ReS2 in addition to the two conventional exciton resonances X1 and X2. Furthermore, for ReS2 we observe two charged excitons (trions) with binding energies of 18 meV and 15 meV, respectively. The bi-excitons of WSe2 become polarization sensitive and inherit polarizing properties from the underlying ReS2 layers, which act as patterned substrates for top layer. Overall, our findings provide a better understanding of optical signatures in 2D anisotropic materials.

Twist Angle Tuning of Moiré Exciton Polaritons in van der Waals Heterostructures.

Twisted atomically thin semiconductors are characterized by moiré excitons. Their optical signatures and selection rules are well understood. However, their hybridization with photons in the strong coupling regime for heterostructures integrated in an optical cavity has not been the focus of research yet. Here, we combine an excitonic density matrix formalism with a Hopfield approach to provide microscopic insights into moiré exciton polaritons. In particular, we show that exciton-light coupling, polariton energy, and even the number of polariton branches can be controlled via the twist angle. We find that these new hybrid light-exciton states become delocalized relative to the constituent excitons due to the mixing with light and higher-energy excitons. The system can be interpreted as a natural quantum metamaterial with a periodicity that can be engineered via the twist angle. Our study presents a significant advance in microscopic understanding and control of moiré exciton polaritons in twisted atomically thin semiconductors.

Valley-exchange coupling probed by angle-resolved photoluminescence.

The optical properties of monolayer transition metal dichalcogenides are dominated by tightly-bound excitons. They form at distinct valleys in reciprocal space, and can interact via the valley-exchange coupling, modifying their dispersion considerably. Here, we predict that angle-resolved photoluminescence can be used to probe the changes of the excitonic dispersion. The exchange-coupling leads to a unique angle dependence of the emission intensity for both circularly and linearly-polarised light. We show that these emission characteristics can be strongly tuned by an external magnetic field due to the valley-specific Zeeman-shift. We propose that angle-dependent photoluminescence measurements involving both circular and linear optical polarisation as well as magnetic fields should act as strong verification of the role of valley-exchange coupling on excitonic dispersion and its signatures in optical spectra.