In this short review, an overview of recent progress in deploying advanced characterization techniques is provided to understand the effects of spatial variation and inhomogeneities in moiré heterostructures over multiple length scales. Particular emphasis is placed on correlating the impact of twist angle misalignment, nano-scale disorder, and atomic relaxation on the moiré potential and its collective excitations, particularly moiré excitons. Finally, future technological applications leveraging moiré excitons are discussed.

UNASSIGNED: Interlayer excitons (IXs), composed of electron and hole states localized in different layers, excel in bilayers composed of atomically thin van der Waals materials such as semiconducting transition-metal dichalcogenides (TMDs) due to drastically enlarged exciton binding energies, exciting spin-valley properties, elongated lifetimes, and large permanent dipoles. The latter allows modification by electric fields and the study of thermalized bosonic quasiparticles, from the single particle level to interacting degenerate dense ensembles. Additionally, the freedom to combine bilayers of different van der Waals materials without lattice or relative twist-angle constraints leads to layer-hybridized and Moiré excitons, which can be widely engineered. This article covers fundamental aspects of IXs, including correlation phenomena as well as the consequence of Moiré superlattices with a strong focus on TMD homo- and heterobilayers.
UNASSIGNED:

Van der Waals heterostructures open up vast possibilities for applications in optoelectronics, especially since it was recognized that the optical properties of transition-metal dichalcogenides (TMDC) can be enhanced by adjacent hBN layers. However, although many micrometer-sized structures have been fabricated, the bottleneck for applications remains the lack of large-area structures with electrically tunable photoluminescence emission. In this study, we demonstrate the electrical charge carrier tuning for large-area epitaxial MoSe2 grown directly on epitaxial hBN. The structure is produced in a multistep procedure involving Metalorganic Vapor Phase Epitaxy (MOVPE) growth of large-area hBN, a wet transfer of hBN onto a SiO2/Si substrate, and the subsequent Molecular Beam Epitaxy (MBE) growth of monolayer MoSe2. The electrically induced change of the carrier concentration is deduced from the evolution of well-resolved charged and neutral exciton intensities. Our findings show that it is feasible to grow large-area, electrically addressable, high-optical-quality van der Waals heterostructures.

Excitons are the neutral quasiparticles that form when Coulomb interactions create bound states between electrons and holes. Due to their bosonic nature, excitons are expected to condense and exhibit superfluidity at sufficiently low temperatures. In interacting Chern insulators, excitons may inherit the nontrivial topology and quantum geometry from the underlying electron wavefunctions. We theoretically investigate the excitonic bound states and superfluidity in flat-band insulators pumped with light. We find that the exciton wavefunctions exhibit vortex structures in momentum space, with the total vorticity being equal to the difference of Chern numbers between the conduction and valence bands. Moreover, both the exciton binding energy and the exciton superfluid density are proportional to the Brillouin-zone average of the quantum metric and the Coulomb potential energy per unit cell. Spontaneous emission of circularly polarized light from radiative decay is a detectable signature of the exciton vorticity. We propose that the vorticity can also be experimentally measured via the nonlinear anomalous Hall effect, whereas the exciton superfluidity can be detected by voltage-drop quantization through a combination of quantum geometry and Aharonov-Casher effect. Topological excitons and their superfluid phase could be realized in flat bands of twisted Van der Waals heterostructures.

Two-dimensional metal halide perovskites are highly versatile for light-driven applications due to their exceptional variety in material composition, which can be exploited for the tunability of mechanical and optoelectronic properties. The band-edge emission is defined by the structure and composition of both organic and inorganic layers, and electron-phonon coupling plays a crucial role in the recombination dynamics. However, the nature of the electron-phonon coupling and what kind of phonons are involved are still under debate. Here we investigate the emission, reflectance, and phonon response from single two-dimensional lead iodide microcrystals with angle-resolved polarized spectroscopy. We find an intricate dependence of the emission polarization with the vibrational directionality in the materials, which reveals that several bands of low-frequency phonons with nonorthogonal directionality contribute to the band-edge emission. Such complex electron-phonon coupling requires adequate models to predict the thermal broadening of the emission and provides opportunities to design polarization properties.

The moiré potential in rotationally misfit two-dimensional (2D) heterostructures has been used to build artificial exciton and electron lattices, which have become platforms for realizing exotic electronic phases. Here, we demonstrate a different approach to create a superlattice potential in 2D crystals by using the near field of an array of polar molecules. A bilayer of titanyl phthalocyanine (TiOPc), consisting of alternating out-of-plane dipoles, is deposited on monolayer MoS2. Time-resolved two-photon photoemission spectroscopy reveals a pair of interlayer exciton states with an energy difference of ∼0.1 eV, which is consistent with the electrostatic potential modulation induced by the TiOPc bilayer as determined by density functional theory calculations. Because the symmetry and the period of this potential superlattice can be changed readily by using molecules of different shapes and sizes, molecule/2D heterostructures can be promising platforms for designing artificial exciton and electron lattices.

The measurement of the electronic bandgap and exciton binding energy in quasi-one-dimensional materials such as carbon nanotubes is challenging due to many-body effects and strong electron-electron interactions. Unlike bulk semiconductors, where the electronic bandgap is well known, the optical resonance in low-dimensional semiconductors is dominated by excitons, making their electronic bandgap more difficult to measure. In this work, we measure the electronic bandgap of networks of polymer-wrapped semiconducting single-walled carbon nanotubes (s-SWCNTs) using non-ideal p-n diodes. We show that our s-SWCNT networks have a short minority carrier lifetime due to the presence of interface trap states, making the diodes non-ideal. We use the generation and recombination leakage currents from these non-ideal diodes to measure the electronic bandgap and excitonic levels of different polymer-wrapped s-SWCNTs with varying diameters: arc discharge (~1.55 nm), (7,5) (0.83 nm), and (6,5) (0.76 nm). Our values are consistent with theoretical predictions, providing insight into the fundamental properties of networks of s-SWCNTs. The techniques outlined here demonstrate a robust strategy that can be applied to measuring the electronic bandgaps and exciton binding energies of a broad variety of nanoscale and quantum-confined semiconductors, including the most modern nanoscale transistors that rely on nanowire geometries.

Anisotropic optical 2D materials are crucial for achieving multiple-quanta functions within quantum materials, which enables the fabrication of axially polarized electronic and optoelectronic devices. In this work, multiple excitonic emissions owning polarization-sensitive orientations are clearly detected in a multilayered quasi-1D ZrS3 nanoribbon with respect to the nanostripe edge. Four excitons denoted as AS1, AS2, AS, and A2 with E ⊥ b polarized direction and one prominent A1 exciton with E || b polarized emission are simultaneously detected in the polarized micro-photoluminescence (µPL) measurement of 1.9-2.2 eV at 10 K. In contrast to light emission, polarized micro-thermoreflectance (µTR) measurements are performed to identify the polarization dependence and verify the excitons in the multilayered ZrS3 nanoribbon from the perspective of light absorption. At 10 K, a prominent and broadened peak on the lower-energy side, containing an indirect resonant emission (DI) observed by µPL and an indirect defect-bound exciton peak (AInd) observed by both µPL and µTR, is simultaneously detected, confirming the existence of a quasi-direct band edge in ZrS3. A van der Waals stacked p-GaSe/n-ZrS3 heterojunction solar cell is fabricated, which demonstrates a maximum axially-polarized conversion efficiency up to 0.412% as the E || b polarized light incident onto the device.

A key challenge in the field of plexcitonic quantum devices is the fabrication of solid-state, device-friendly plexcitonic nanostructures using inexpensive and scalable techniques. Lithography-free, bottom-up nanofabrication methods have remained relatively unexplored within the context plexcitonic coupling. In this work, a plexcitonic system consisting of thermally dewetted plasmonic gold nanoislands (AuNI) coated with a thin film of J-aggregates was investigated. Control over nanoisland size and morphology allowed for a range of plasmon resonances with variable detuning from the exciton. The extinction spectra of the hybrid AuNI/J-aggregate films display clear splitting into upper and lower hybrid resonances, while the dispersion curve shows anti-crossing behavior with an estimated Rabi splitting of 180 eV at zero detuning. As a proof of concept for quantum sensing, the AuNI/J-aggregate hybrid was demonstrated to behave as a plexcitonic sensor for hydrochloric acid vapor analyte. This work highlights the possibility of using thermally dewetted nanoparticles as a platform for high-quality, tunable, cost-effective, and scalable plexcitonic nanostructures for sensing devices and beyond.

Heterostructures (HSs) formed by the transition-metal dichalcogenide materials have shown great promise in next-generation (opto)electronic applications. An artificially twisted HS allows us to manipulate the optical and electronic properties. In this work, we introduce the understanding of the energy transfer (ET) process governed by the dipolar interaction in a twisted molybdenum diselenide (MoSe2) homobilayer without any charge-blocking interlayer. We fabricated an unconventional homobilayer (i.e., HS) with a large twist angle (∼57°) by combining the chemical vapor deposition (CVD) and mechanical exfoliation (Exf.) techniques to fully exploit the lattice parameter mismatch and indirect/direct (CVD/Exf.) bandgap nature. These effectively weaken the interlayer charge transfer and allow the ET to control the carrier recombination channels. Our experimental and theoretical results explain a massive HS photoluminescence enhancement due to an efficient ET process. This work shows that the electronically decoupled MoSe2 homobilayer is coupled by the ET process, mimicking a \"true\" heterobilayer nature.