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 in 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.
Moiré interlayer exciton in transition metal dichalcogenide heterobilayer features a permanent electric dipole that enables the electrostatic control of its flow, and optical dipole that is spatially varying in the moiré landscape. We show the hybridization of moiré interlayer exciton with photons in a planar 2D cavity leads to two types of moiré polaritons that exhibit distinct forms of topological transport phenomena including the spin/valley Hall and polarization Hall effects, which feature remarkable electrical tunability through the control of exciton-cavity detuning by the interlayer bia…
Two-dimensional van der Waals (vdW) crystals can sustain various types of polaritons with strong electromagnetic confinements, making them highly attractive for the nanoscale photonic and optoelectronic applications. While extensive experimental and numerical studies are devoted to the polaritons of the vdW crystals, analytical models are sparse. Particularly, applying such a model to describe the polariton behaviors visualized by state-of-art near-field optical microscopy requires further investigation. Herein, we develop an analytical waveguide model to describe the polariton propagations in…
Moiré lattices formed from semiconductor bilayers host tightly localised excitons that can simultaneously couple strongly to light and possess large electric dipole moments. This facilitates the realization of new forms of polaritons that are very strongly interacting and that have been predicted to lead to strong optical nonlinearities controlled by multi-photon resonances. Here, we investigate the role of the non-local component of the exciton-exciton (dipolar) interactions on the optical response of these strongly-interacting moiré exciton-polaritons under conditions of strong optical drivi…
Van der Waals heterostructures of graphene and hexagonal boron nitride feature a moiré superlattice for graphene's Dirac electrons. Here, we review the effects generated by this superlattice, including a specific miniband structure featuring gaps and secondary Dirac points, and a fractal spectrum of magnetic minibands known as Hofstadter's butterfly.
Twisted two-dimensional bi-layers offer exquisite control on the electronic bandstructure through the interlayer rotation and coupling, enabling magic-angle flat-band superconductivity and moiré excitons. Here, we demonstrate how analogous principles, combined with large anisotropy, enable extreme control and manipulation of the photonic dispersion of phonon polaritons (PhPs) in van der Waals (vdW) bi-layers. We experimentally observe tunable topological transitions from open (hyperbolic) to closed (elliptic) dispersion contours in twisted bi-layered α-MoO3 at photonic magic angles, induced by…
Different atomistic registry between the layers forming the inner and outer nanotubes can form one-dimensional (1D) van der Waals (vdW) moiré superlattices. Unlike the two-dimensional (2D) vdW moiré superlattices, effects of 1D vdW moiré superlattices on electronic and optical properties in 1D moiré superlattices are not well understood, and they are often neglected. In this Perspective, we summarize new experimental observations and theoretical perspectives related to interlayer interactions in double-walled carbon nanotubes (DWNTs), a representative 1D vdW moiré system. Our discussion will f…
We consider the role of deformations in graphene heterostructures with hexagonal crystals (including strain, wrinkles and dislocations) on the geometrical properties of moire patterns characteristic for a pair of two incommensurate misaligned isostructural crystals. By, employing a phenomenological theory to describe generic moire perturbation in van der Waals heterostructures of graphene and hexagonal crystals we investigate the electronic properties of such heterostructure.
Controlling matter-light interactions with cavities is of fundamental importance in modern science and technology. It is exemplified in the strong-coupling regime, where matter-light hybrid modes form, with properties controllable via the photon component on the optical-wavelength scale. In contrast, matter excitations on the nanometer scale are harder to access. In two-dimensional van der Waals heterostructures, a tunable moiré lattice potential for electronic excitations may form, enabling correlated electron gases in lattice potentials. Excitons confined in moiré lattices have also been rep…
Phonon polaritons (PhPs),light coupled to lattice vibrations,with in-plane hyperbolic dispersion exhibit ray-like propagation with large wavevectors and enhanced density of optical states along certain directions on a surface. As such, they have raised a surge of interest as they promise unprecedented possibilities for the manipulation of infrared light with planar circuitry and at the nanoscale. Here, we demonstrate, for the first time, the focusing of in-plane hyperbolic PhPs propagating along thin slabs of MoO3. To that end, we developed metallic nanoantennas of convex geometries for both t…
Van der Waals heterostructures assembled from layers of 2D materials have attracted considerable interest due to their novel optical and electrical properties. Here we report a scattering-type scanning near field optical microscopy study of hexagonal boron nitride on black phosphorous (h-BN/BP) heterostructures, demonstrating the first direct observation of in-plane anisotropic phonon polariton modes in vdW heterostructures. Strikingly, the measured in-plane optical anisotropy along armchair and zigzag crystal axes exceeds the ratio of refractive indices of BP in the x-y plane. We explain that…
The spatial dependence of the van der Waals (vdW) energy between graphene and hexagonal boron-nitride (h-BN) is investigated using atomistic simulations. The van der Waals energy between graphene and h-BN shows a hexagonal superlattice structure identical to the observed Moiré pattern in the local density of states (LDOS) which depends on the lattice mismatch and misorientation angle between graphene and h-BN. Our results provide atomistic features of the weak van der Waals interaction between graphene and BN which are in agreement with experiment and provide an analytical expression for the s…
Stacking monolayers of transition metal dichalcogenides into a heterostructure with a finite twist-angle gives rise to artificial moiré 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 moiré exciton resonances has not been fully clarified yet. Here, we combine first principle calculations with the excitonic density matrix formalism to study transitions…
Formation of moiré superlattices is common in Van der Waals heterostructures as a result of the mismatch between lattice constants and misalignment of crystallographic directions of the constituent two-dimensional crystals. We discuss theoretically electron transport in a Van der Waals tunnelling transistor in which one of the electrodes is made of two crystals forming a moiré superlattice at their interface. By investigating structures containing either the aligned graphene/hexagonal boron nitride heterostructure or twisted bilayer graphene, we show that negative differential resistance is po…
The emergence of a topological superconducting state in van der Waals heterostructures provides a new platform for exploring novel strategies to control topological superconductors. In particular, impurities in van der Waals heterostructures, generically featuring a moire pattern, can potentially lead to the unique interplay between atomic and moire length scales, a feature absent in generic topological superconductors. Here we address the impact of non-magnetic impurities on a topological moire superconductor, both in the weak and strong regime, considering both periodic arrays and single imp…
van der Waals nanomaterials supporting phonon polariton quasiparticles possess unprecedented light confinement capabilities, making them ideal systems for molecular sensing, thermal emission, and subwavelength imaging applications, but they require defect-free crystallinity and nanostructured form factors to fully showcase these capabilities. We introduce bottom-up-synthesized α-MoO3 structures as nanoscale phonon polaritonic systems that feature tailorable morphologies and crystal qualities consistent with bulk single crystals. α-MoO3 nanoribbons serve as low-loss hyperbolic Fabry-Pérot nanor…
The incommensurate stacking of multi-layered two-dimensional materials is a challenging problem from a theoretical perspective and an intriguing avenue for manipulating their physical properties. Here we present a multi-scale model to obtain the mechanical relaxation pattern of twisted trilayer van der Waals (vdW) heterostructures with two independent twist angles, a generally incommensurate system without a supercell description. We adopt the configuration space as a natural description of such incommensurate layered materials, based on the local environment of atomic positions, bypassing the…
yperbolic polaritons in van der Waals materials recently attract a lot of attention, owing to their strong electromagnetic field confinement, ultraslow group velocities and long lifetimes. Typically, volume confined hyperbolic polaritons (HPs) are studied. Here we show the first near-field optical images of hyperbolic surface polarities, HSPs, which are confined and guided at the edges of thin flakes of a vdW material. To that end, we applied scattering-type scanning near-field optical microscopy (s-SNOM) for launching and real-space nanoimaging of hyperbolic surface phonon polariton modes on …
We explore the skyrmion formation and control possibilities in 2D magnets from the ubiquitous moiré pattern in vdW heterostructures. Using the example of a ferromagnetic monolayer on an antiferromagnetic substrate, we demonstrate a new origin of skyrmions in the 2D magnets, from the lateral modulation of interlayer magnetic coupling by the locally different atomic registries in moiré. The moiré skyrmions are doubly degenerate with opposite topological charge, and trapped at an ordered array of sites with the moiré periodicity that can be dramatically tuned by strain and interlayer translation.…
Highly nonlinear Moiré exciton and trion polaritons
Laboratory for Physical Sciences, University of Maryland（马里兰大学物理科学实验室）；University of Rochester（罗切斯特大学）；University of Notre Dame（圣母大学）；The Institute of Optics, University of Rochester（罗切斯特大学光学研究所）
In van der Waals (vdW) heterostructures formed by stacking two monolayer semiconductors, lattice mismatch or rotational misalignment introduces an in-plane moiré superlattice. While it is widely recognized that a moiré 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 moiré potential in a high-quality MoSe…
We investigate the magnetic proximity effect in van der Waals heterostructure formed by a monolayer semiconductor stacked on a 2D ferromagnet, where the lattice mismatch and twisting between the layers typically lead to the formation of moiré pattern. We find that the magnetic proximity effect arising from the spin dependent interlayer coupling depends sensitively on the interlayer atomic registry. Consequently, in the moiré pattern, the spatial variation of the atomic registry leads to a lateral modulation of magnetic proximity field. Such moiré modulated magnetic proximity effect manifests a…
Charge Tunable Optical Nonlinearity of Moiré Exciton-Polaritons
Carl von Ossietzky Universität Oldenburg（奥尔登堡卡尔·冯·奥西埃茨基大学）；Xiamen University Malaysia（厦门大学马来西亚分校）；Friedrich-Schiller University Jena（耶拿弗里德里希·席勒大学）；Fraunhofer-Institute for Applied Optics and Precision Engineering IOF（弗劳恩霍夫应用光学和精密工程研究所IOF）；National Institute for Materials Science（国立材料研究所）；Julius-Maximilians-Universität Würzburg（维尔茨堡朱利叶斯-马克西米利安大学）；Ludwig-Maximilians-Universität München（慕尼黑路德维希-马克西米利安大学）
We investigated experimentally the valley Zeeman splitting of excitonic peaks in the photoluminescence (PL) spectra of high-quality hBN/WS2/MoSe2/hBN heterostructures at near-zero twist angles under perpendicular magnetic fields up to 20 T. We identify two neutral exciton peaks in the PL spectra: the lower energy one exhibits a reduced g-factor relative to that of the higher energy peak, and much lower than the recently reported values for interlayer excitons in other van der Waals (vdW) heterostructures. We provide evidence that such a discernible g-factor stems from the spatial confinement o…
The optical and electronic properties of van der Waals (vdW) heterostructures depend strongly on the atomic stacking order of the constituent layers. This is exemplified by periodic variation of the local atomic registry, known as moire patterns, giving rise to superconductivity and ferromagnetism in twisted bilayer graphene and novel exciton states in transition metal dichalcogenides (TMD) heterobilayers. However, the presence of the nanometer-scale moire superlattices is typically deduced indirectly, because conventional imaging techniques, such as transmission electron microscopy (TEM), req…
The properties of van der Waals (vdW) heterostructures are drastically altered by a tunable moiré 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 moiré crystal with a large supercell size and deep potential, interlayer excitons may be completely localized. As the…
Electromagnetic field confinement is crucial for nanophotonic technologies, since it allows for enhancing light-matter interactions, thus enabling light manipulation in deep sub-wavelength scales. In the terahertz (THz) spectral range, radiation confinement is conventionally achieved with specially designed metallic structures - such as antennas or nanoslits - with large footprints due to the rather long wavelengths of THz radiation. In this context, phonon polaritons - light coupled to lattice vibrations - in van der Waals (vdW) crystals have emerged as a promising solution for controlling li…
Optical nanoresonators are fundamental building blocks in a number of nanotechnology applications (e.g. in spectroscopy) due to their ability to efficiently confine light at the nanoscale. Recently, nanoresonators based on the excitation of phonon polaritons (PhPs) $-$ light coupled to lattice vibrations $-$ in polar crystals (e.g. SiC, or h-BN) have attracted much attention due to their strong field confinement, high-quality factors, and potential to enhance the photonic density of states at mid-infrared (IR) frequencies. Here, we go one step further by introducing PhPs nanoresonators that no…
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 moiré superlattice. Its presence in graphene/hexagonal boron nitride (hBN) structures led to the observation of electronic minibands, whereas its effect enhanced by …
The large oscillator strength of excitons in transition metal dichalcogenide layers facilitates the formation of exciton-polariton resonances for monolayers and van-der-Waals heterostructures embedded in optical microcavities. Here, we show, that locally changing the number of layers in a WSe2/hBN/WSe2 van-der-Waals heterostructure embedded in a monolithic, high-quality-factor cavity gives rise to a local variation of the coupling strength. This effect yields a polaritonic stair case potential, which we demonstrate at room temperature. Our result paves the way towards engineering local polarit…
Moire engineering as a configuration method to twist van der Waals materials has delivered a series of advances in electronics, magnetics and optics. Yet these advances stem from peculiar moire superlattices which form at small specific twisting angles. Here we report the configuration of nanoscale light-matter waves-the polaritons-by twisting stacked $α$-phase molybdenum trioxide $α$-MoO3 slabs in the broad range of 0$^o$ to 90$^o$. Our combined experimental and theoretical results reveal a variety of polariton wavefront geometry and topological transitions via the twisting. The polariton twi…
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 moiré superlattice encodes elusive insights into the local interlayer interaction. Here we introduce moiré metrology as a combined experiment-theory framework to probe the stacking energy landscape of bilayer structures at the 0.1 me…
Moiré superlattices open an unprecedented opportunity for tailoring interactions between quantum particles and their coupling to electromagnetic fields. Strong superlattice potential generates moiré minibands of excitons -- bound pairs of electrons and holes that reside either in a single layer (intralayer excitons) or two separate layers (interlayer excitons). The twist-angle-controlled interlayer hybridization of carriers can also mix the two types of excitons to combine the strengths of both. Here, we report a direct observation of spatially mixed moiré excitons in angle-aligned WSe2/WS2 an…
Quantum spin-liquid van der Waals magnets such as TaS$_2$, TaSe$_2$, and RuCl$_3$ provide a natural platform to explore new exotic phenomena associated with spinon physics, whose properties can be controlled by exchange proximity with ferromagnetic insulators such as CrBr$_3$. Here we put forward a twisted van der Waals heterostructure based on a quantum spin-liquid bilayer encapsulated between ferromagnetic insulators. We demonstrate the emergence of spinon flat bands and topological spinon states in such heterostructure, where the emergence of a topological gap is driven by the twist. We fur…
Layered materials can be assembled vertically to fabricate a new class of van der Waals (VDW) heterostructures a few atomic layers thick, compatible with a wide range of substrates and optoelectronic device geometries, enabling new strategies for control of light-matter coupling. Here, we incorporate molybdenum diselenide/boron nitride (MoSe$_2$/hBN) quantum wells (QWs) in a tunable optical microcavity. Part-light-part-matter polariton eigenstates are observed as a result of the strong coupling between MoSe$_2$ excitons and cavity photons, evidenced from a clear anticrossing between the neutra…
Van der Waals materials and heterostructures manifesting strongly bound room temperature exciton states exhibit emergent physical phenomena and are of a great promise for optoelectronic applications. Here, we demonstrate that nanostructured multilayer transition metal dichalcogenides by themselves provide an ideal platform for excitation and control of excitonic modes, paving the way to exciton-photonics. Hence, we show that by patterning the TMDCs into nanoresonators, strong dispersion and avoided crossing of excitons and hybrid polaritons with interaction potentials exceeding 410 meV may be …
