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The enhanced Coulomb interaction in two-dimensional (2D) semiconductors leads to the tightly bound electron-hole pairs known as excitons. The large binding energy of excitons enables the formation of Rydberg excitons with high principal quantum numbers (n), analogous to Rydberg atoms. Rydberg excitons possess strong interactions among themselves, as well as sensitive responses to external stimuli. Here, we probe Rydberg exciton resonances through photocurrent spectroscopy in a monolayer WSe2 p-n junction formed by a split-gate geometry. We show that an external in-plane electric field not only induces a large Stark shift of Rydberg excitons up to quantum principal number n=3 but also mixes different orbitals and brightens otherwise dark states such as 3p and 3d. Our study provides an exciting platform for engineering Rydberg excitons for new quantum states and quantum sensing.

Moir\'e superlattices of semiconducting transition metal dichalcogenides (TMDCs) enable unprecedented spatial control of electron wavefunctions in an artificial lattice with periodicities more than ten times larger than that of atomic crystals, leading to emerging quantum states with fascinating electronic and optical properties. The breaking of translational symmetry further introduces a new degree of freedom inside each moir\'e unit cell: high symmetry points of energy minima called moir\'e sites, behaving as spatially separated quantum dots. The superposition of a quasiparticle wavefunction between different moir\'e sites will enable a new platform for quantum information processing but is hindered by the suppressed electron tunneling between moir\'e sites. Here we demonstrate the superposition between two moir\'e sites by constructing an angle-aligned trilayer WSe2/monolayer WS2 moir\'e heterojunction. The two moir\'e sites with energy minimum allow the formation of two different interlayer excitons, with the hole residing in either moir\'e site of the first WSe2 layer interfacing the WS2 layer and the electron in the third WSe2 layer. An external electric field can drive the hybridization of either of the interlayer excitons with the intralayer excitons in the third WSe2 layer, realizing the continuous tuning of interlayer exciton hopping between two moir\'e sites. Therefore, a superposition of the two interlayer excitons localized at different moir\'e sites can be realized, which can be resolved in the electric-field-dependent optical reflectance spectra, distinctly different from that of the natural trilayer WSe2 in which the moir\'e modulation is absent. Our study illustrates a strategy of harnessing the new moir\'e site degree of freedom for quantum information science, a new direction of twistronics.

Strongly enhanced electron-electron interaction in semiconducting moir\'e superlattices formed by transition metal dichalcogenides (TMDCs) heterobilayers has led to a plethora of intriguing fermionic correlated states. Meanwhile, interlayer excitons in a type-II aligned TMDC heterobilayer moir\'e superlattice, with electrons and holes separated in different layers, inherit this enhanced interaction and strongly interact with each other, promising for realizing tunable correlated bosonic quasiparticles with valley degree of freedom. We employ photoluminescence spectroscopy to investigate the strong repulsion between interlayer excitons and correlated electrons in a WS2/WSe2 moir\'e superlattice and combine with theoretical calculations to reveal the spatial extent of interlayer excitons and the band hierarchy of correlated states. We further find that an excitonic Mott insulator state emerges when one interlayer exciton occupies one moir\'e cell, evidenced by emerging photoluminescence peaks under increased optical excitation power. Double occupancy of excitons in one unit cell requires overcoming the energy cost of exciton-exciton repulsion of about 30-40 meV, depending on the stacking configuration of the WS2/WSe2 heterobilayer. Further, the valley polarization of the excitonic Mott insulator state is enhanced by nearly one order of magnitude. Our study demonstrates the WS2/WSe2 moir\'e superlattice as a promising platform for engineering and exploring new correlated states of fermion, bosons, and a mixture of both.

Moir\'e superlattices of transitional metal dichalcogenides exhibit strong electron-electron interaction that has led to experimental observations of Mott insulators and generalized Wigner crystals. In this letter, we report direct measurements of the thermodynamic gaps of these correlated insulating states in a dual-gate WS2/WSe2 moir\'e bilayer. We employ the microwave impedance microscopy to probe the electronic features in both the graphene top gate and the moir\'e bilayer, from which we extract the doping dependence of the chemical potential of the moir\'e bilayer and the energy gaps for various correlated insulating states utilizing the Landau quantization of graphene. These gaps are relatively insensitive to the application of an external electric field to the WS2/WSe2 moir\'e bilayer.

Transition metal dichalcogenide (TMDC) moir\'e superlattices, owing to the moir\'e flatbands and strong correlation, can host periodic electron crystals and fascinating correlated physics. The TMDC heterojunctions in the type-II alignment also enable long-lived interlayer excitons that are promising for correlated bosonic states, while the interaction is dictated by the asymmetry of the heterojunction. Here we demonstrate a new excitonic state, quadrupolar exciton, in a symmetric WSe2-WS2-WSe2 trilayer moir\'e superlattice. The quadrupolar excitons exhibit a quadratic dependence on the electric field, distinctively different from the linear Stark shift of the dipolar excitons in heterobilayers. This quadrupolar exciton stems from the hybridization of WSe2 valence moir\'e flatbands. The same mechanism also gives rise to an interlayer Mott insulator state, in which the two WSe2 layers share one hole laterally confined in one moir\'e unit cell. In contrast, the hole occupation probability in each layer can be continuously tuned via an out-of-plane electric field, reaching 100% in the top or bottom WSe2 under a large electric field, accompanying the transition from quadrupolar excitons to dipolar excitons. Our work demonstrates a trilayer moir\'e system as a new exciting playground for realizing novel correlated states and engineering quantum phase transitions.

In the archetypal monolayer semiconductor WSe$_2$, the distinct ordering of spin-polarized valleys (low-energy pockets) in the conduction band allows for studies of not only simple neutral excitons and charged excitons (i.e., trions), but also more complex many-body states that are predicted at higher electron densities. We discuss magneto-optical measurements of electron-rich WSe$_2$ monolayers, and interpret the spectral lines that emerge at high electron doping as optical transitions of 6-body exciton states ("hexcitons") and 8-body exciton states ("oxcitons"). These many-body states emerge when a photoexcited electron-hole pair interacts simultaneously with multiple Fermi seas, each having distinguishable spin and valley quantum numbers. In addition, we identify the energies of primary and satellite optical transitions of hexcitons in the photoluminescence spectrum.

Despite the broadband response, limited optical absorption at a particular wavelength hinders the development of optoelectronics based on Dirac fermions. Heterostructures of graphene and various semiconductors have been explored for this purpose, while non-ideal interfaces often limit the performance. The topological insulator is a natural hybrid system, with the surface states hosting high-mobility Dirac fermions and the small-bandgap semiconducting bulk state strongly absorbing light. In this work, we show a large photocurrent response from a field effect transistor device based on intrinsic topological insulator Sn-Bi1.1Sb0.9Te2S. The photocurrent response is non-volatile and sensitively depends on the initial Fermi energy of the surface state, and it can be erased by controlling the gate voltage. Our observations can be explained with a remote photo-doping mechanism, in which the light excites the defects in the bulk and frees the localized carriers to the surface state. This photodoping modulates the surface state conductivity without compromising the mobility, and it also significantly modify the quantum Hall effect of the surface state. Our work thus illustrates a route to reversibly manipulate the surface states through optical excitation, shedding light into utilizing topological surface states for quantum optoelectronics.

Moir\'e superlattices of van der Waals materials, such as twisted graphene and transitional metal dichalcogenides, have recently emerged as a fascinating platform to study strongly correlated states in two dimensions, thanks to the strong electron interaction in the moir\'e minibands. In most systems, the correlated states appear when the moir\'e lattice is filled by integer number of electrons per moir\'e unit cell. Recently, correlated states at fractional fillings of 1/3 and 2/3 holes per moir\'e unit cell has been reported in the WS2/WSe2 heterobilayer, hinting the long range nature of the electron interaction. In this work, employing a scanning microwave impedance microscopy technique that is sensitive to local electrical properties, we observe a series of correlated insulating states at fractional fillings of the moir\'e minibands on both electron- and hole-doped sides in angle-aligned WS2/WSe2 hetero-bilayers, with certain states persisting at temperatures up to 120 K. Monte Carlo simulations reveal that these insulating states correspond to ordering of electrons in the moir\'e lattice with a periodicity much larger than the moir\'e unit cell, indicating a surprisingly strong and long-range interaction beyond the nearest neighbors. Our findings usher in unprecedented opportunities in the study of strongly correlated states in two dimensions.

Monolayer transition metal dichalcogenides (TMDs) are the first truly two-dimensional (2D) semiconductor, providing an excellent platform to investigate light-matter interaction in the 2D limit. Apart from fundamental scientific exploration, this material system has attracted active research interest in the nanophotonic devices community for its unique optoelectronic properties. The inherently strong excitonic response in monolayer TMDs can be further enhanced by exploiting the temporal confinement of light in nanophotonic structures. Dielectric metasurfaces are one such two-dimensional nanophotonic structures, which have recently demonstrated strong potential to not only miniaturize existing optical components, but also to create completely new class of designer optics. Going beyond passive optical elements, researchers are now exploring active metasurfaces using emerging materials and the utility of metasurfaces to enhance the light-matter interaction. Here, we demonstrate a 2D exciton-polariton system by strongly coupling atomically thin tungsten diselenide (WSe2) monolayer to a silicon nitride (SiN) metasurface. Via energy-momentum spectroscopy of the WSe2-metasurface system, we observed the characteristic anti-crossing of the polariton dispersion both in the reflection and photoluminescence spectrum. A Rabi splitting of 18 meV was observed which matched well with our numerical simulation. The diffraction effects of the nano-patterned metasurface also resulted in a highly directional polariton emission. Finally, we showed that the Rabi splitting, the polariton dispersion and the far-field emission pattern could be tailored with subwavelength-scale engineering of the optical meta-atoms. Our platform thus opens the door for the future development of novel, exotic exciton-polariton devices by advanced meta-optical engineering.

Despite inherently poor interlayer conductivity, photodetectors made from few-layer devices of 2D transition metal dichalcogenides (TMDs) such as WSe$_2$ and MoS$_2$ can still yield a desirably fast ($\leq$90 ps) and efficient ($\epsilon$$>$40\%) photoresponse. By combining ultrafast photocurrent (U-PC) and transient absorption (TA) microscopy, the competing electronic escape and recombination rates are unambiguously identified in otherwise complex kinetics. Both the U-PC and TA response of WSe$_2$ yield matching interlayer electronic escape times that accelerate from 1.6 ns to 86 ns with applied $E$-field to predict the maximum device PC-efficiency realized of $\sim$44\%. The slope of the escape rates versus $E$-field suggests out-of-plane electron and hole mobilities of 0.129 and 0.031 cm$^2$/V$s$ respectively. Above $\sim$10$^{11}$ photons/cm$^{2}$ incident flux, defect-assisted Auger scattering greatly decreases efficiency by trapping carriers at vacancy defects. Both TA and PC spectra identify a metal-vacancy sub-gap peak with $\sim$5.6 ns lifetime as a primary trap capturing carriers as they hop between layers. Synchronous TA and U-PC microscopy show the\ net PC collected is modelled by a kinetic rate-law of electronic escape competing against the linear and nonlinear Auger recombination rates. This simple rate-model further predicts the PC-based dynamics, nonlinear amplitude and efficiency, $\epsilon$ over a 10$^5$ range of incident photon flux in few-layer WSe$_2$ and MoS$_2$ devices., Comment: 10 pages, 4 figures

Single molecular electrets exhibiting single molecule electric polarization switching have been long desired as a platform for extremely small non-volatile storage devices, although it is controversial because of the poor stability of single molecular electric dipoles. Here we study the single molecular device of GdC82, where the encapsulated Gd atom forms a charge center, and we have observed a gate controlled switching behavior between two sets of single electron transport stability diagrams. The switching is operated in a hysteresis loop with a coercive gate field of around 0.5Vnm. Theoretical calculations have assigned the two conductance diagrams to corresponding energy levels of two states that the Gd atom is trapped at two different sites of the C82 cage, which possess two different permanent electrical dipole orientations. The two dipole states are stabilized by the anisotropic energy and separated by a transition energy barrier of 70 meV. Such switching is then accessed to the electric field driven reorientation of individual dipole while overcoming the barriers by the coercive gate field, and demonstrates the creation of a single molecular electret.

Transition metal dichalcogenides (TMDCs) heterostructure with a type II alignment hosts unique interlayer excitons with the possibility of spin-triplet and spin-singlet states. However, the associated spectroscopy signatures remain elusive, strongly hindering the understanding of the Moire potential modulation of the interlayer exciton. In this work, we unambiguously identify the spin-singlet and spin-triplet interlayer excitons in the WSe2/MoSe2 hetero-bilayer with a 60-degree twist angle through the gate- and magnetic field-dependent photoluminescence spectroscopy. Both the singlet and triplet interlayer excitons show giant valley-Zeeman splitting between the K and K' valleys, a result of the large Lande g-factor of the singlet interlayer exciton and triplet interlayer exciton, which are experimentally determined to be ~ 10.7 and ~ 15.2, respectively, in good agreement with theoretical expectation. The PL from the singlet and triplet interlayer excitons show opposite helicities, determined by the atomic registry. Helicity-resolved photoluminescence excitation (PLE) spectroscopy study shows that both singlet and triplet interlayer excitons are highly valley-polarized at the resonant excitation, with the valley polarization of the singlet interlayer exciton approaches unity at ~ 20 K. The highly valley-polarized singlet and triplet interlayer excitons with giant valley-Zeeman splitting inspire future applications in spintronics and valleytronics.

Organic-inorganic halide perovskites are intrinsically unstable when exposed to moisture and/or light. Additionally, the presence of lead in many perovskites raises toxicity concerns. Herein is reported a thin film of BaZrS3, a lead-free chalcogenide perovskite. Photoluminescence and X-ray diffraction measurements show that BaZrS3 is far more stable than methylammonium lead iodide (MAPbI3) in moist environments. Moisture- and light-induced degradations in BaZrS3 and MAPbI3 are compared by using simulations and calculations based on density functional theory. The simulations reveal drastically slower degradation in BaZrS3 due to two factors - weak interaction with water, and very low rates of ion migration. BaZrS3 photo-detecting devices with photo-responsivity of ~46.5 mA W-1 are also reported. The devices retain ~60% of their initial photo-response after 4 weeks in ambient conditions. Similar MAPbI3 devices degrade rapidly and show ~95% decrease in photo-responsivity in just 4 days. The findings establish the superior stability of BaZrS3 and strengthen the case for its use in optoelectronics. New possibilities for thermoelectric energy conversion using these materials are also demonstrated.

Inversion symmetry breaking and three-fold rotation symmetry grant the valley degree of freedom to the robust exciton in monolayer transition metal dichalcogenides (TMDCs), which can be exploited for valleytronics applications. However, the short lifetime of the exciton significantly constrains the possible applications. In contrast, dark exciton could be long-lived but does not necessarily possess the valley degree of freedom. In this work, we report the identification of the momentum-dark, intervalley exciton in monolayer WSe2 through low-temperature magneto-photoluminescence (PL) spectra. Interestingly, the intervalley exciton is brightened through the emission of a chiral phonon at the corners of the Brillouin zone (K point), and the pseudoangular momentum (PAM) of the phonon is transferred to the emitted photon to preserve the valley information. The chiral phonon energy is determined to be ~ 23 meV, based on the experimentally extracted exchange interaction (~ 7 meV), in excellent agreement with the theoretical expectation of 24.6 meV. The long-lived intervalley exciton with valley degree of freedom adds an exciting quasiparticle for valleytronics, and the coupling between the chiral phonon and intervalley exciton furnishes a venue for valley spin manipulation.