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Register a new userMoire Excitons in Van der Waals Heterostructures
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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.
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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.
Atomically-thin layers of two-dimensional materials can be assembled in vertical stacks held together by relatively weak van der Waals forces, allowing for coupling between monolayer crystals with incommensurate lattices and arbitrary mutual rotation. A profound consequence of using these degrees of freedom is the emergence of an overarching periodicity in the local atomic registry of the constituent crystal structures, known as a moire superlattice. Its presence in graphene/hexagonal boron nitride (hBN) structures led to the observation of electronic minibands, whereas its effect enhanced by interlayer resonant conditions in twisted graphene bilayers culminated in the observation of the superconductor-insulator transition at magic twist angles. Here, we demonstrate that, in semiconducting heterostructures built of incommensurate MoSe2 and WS2 monolayers, excitonic bands can hybridise, resulting in the resonant enhancement of the moire superlattice effects. MoSe2 and WS2 are specifically chosen for the near degeneracy of their conduction band edges to promote the hybridisation of intra- and interlayer excitons, which manifests itself through a pronounced exciton energy shift as a periodic function of the interlayer rotation angle. This occurs as hybridised excitons (hX) are formed by holes residing in MoSe2 bound to a twist-dependent superposition of electron states in the adjacent monolayers. For heterostructures with almost aligned pairs of monolayer crystals, resonant mixing of the electron states leads to pronounced effects of the heterostructures geometrical moire pattern on the hX dispersion and optical spectrum. Our findings underpin novel strategies for band-structure engineering in semiconductor devices based on van der Waals heterostructures.
The emerging field of twistronics, which harnesses the twist angle between two-dimensional materials, represents a promising route for the design of quantum materials, as the twist-angle-induced superlattices offer means to control topology and strong correlations. At the small twist limit, and particularly under strain, as atomic relaxation prevails, the emergent moire superlattice encodes elusive insights into the local interlayer interaction. Here we introduce moire metrology as a combined experiment-theory framework to probe the stacking energy landscape of bilayer structures at the 0.1 meV/atom scale, outperforming the gold-standard of quantum chemistry. Through studying the shapes of moire domains with numerous nano-imaging techniques, and correlating with multi-scale modelling, we assess and refine first-principle models for the interlayer interaction. We document the prowess of moire metrology for three representative twisted systems: bilayer graphene, double bilayer graphene and H-stacked $MoSe_2/WSe_2$. Moire metrology establishes sought after experimental benchmarks for interlayer interaction, thus enabling accurate modelling of twisted multilayers.
We report an experimental study of excitons in a double quantum well van der Waals heterostructure made of atomically thin layers of Mo* and hexagonal boron nitride (hBN). The emission of neutral and charged excitons is controlled by gate voltage, temperature, and both the helicity and the power of optical excitation.
Indirect excitons (IXs) in van der Waals transition-metal dichalcogenide (TMD) heterostructures are characterized by a high binding energy making them stable at room temperature and giving the opportunity for exploring fundamental phenomena in excitonic systems and developing excitonic devices operational at high temperatures. We present the observation of IXs at room temperature in van der Waals TMD heterostructures based on monolayers of MoS$_2$ separated by atomically thin hexagonal boron nitride. The IXs realized in the TMD heterostructure have lifetimes orders of magnitude longer than lifetimes of direct excitons in single-layer TMD, and their energy is gate controlled.
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