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Dielectric engineering of heterostructures made from two-dimensional van der Waals semiconductors is a unique and powerful tool to tailor the electric and optical band gaps solely via the dielectric environment and the crystal thickness modulation. Here, we utilize high quality MoTe2 monolayer and bilayer crystals as a candidate for near-infrared photonic applications. The crystals are exfoliated on various technologically relevant carrier substrates: silicon/silicon dioxide, poly(methyl methacrylate), hexagonal boron nitride, silicon carbide, and silicon nitride. These substrates provide a large range of high frequency dielectric constants from 2.1 to 7.0 for MoTe2-containing heterostructures. We assess the relationship between the environmental dielectric function and Coulomb screening by combining detailed spectroscopic measurements, utilizing low-temperature and high-spatially resolved photoluminescence and contrast reflectivity, with microscopic many-body modeling, to explore the potential of this less-recognized material platform for applications in optoelectronics at photon wavelengths above 1 μm. We observe a redshift of the optical gap emission energy from the monolayer to bilayer regime on the order of 30 meV. Furthermore, the thickness controlled shift is slightly larger than the one induced by the local dielectric environment, which ranges on the order of 20 meV for the MoTe2 monolayers and on the order of 8 meV for the MoTe2 bilayers. We also show that the local dielectric screening barely affects the trion binding energy, which is captured by our microscopic model, accounting for the screened Coulomb potential for the heterostructures. [ABSTRACT FROM AUTHOR]

Modulated reflectance (contactless electroreflectance (CER), photoreflectance (PR), and piezoreflectance (PzR)) has been applied to study direct optical transitions in bulk MoS2, MoSe2, WS2, and WSe2. In order to interpret optical transitions observed in CER, PR, and PzR spectra, the electronic band structure for the four crystals has been calculated from the first principles within the density functional theory for various points of Brillouin zone including K and H points. It is clearly shown that the electronic band structure at H point of Brillouin zone is very symmetric and similar to the electronic band structure at K point, and therefore, direct optical transitions at H point should be expected in modulated reflectance spectra besides the direct optical transitions at the K point of Brillouin zone. This prediction is confirmed by experimental studies of the electronic band structure of MoS2, MoSe2, WS2, and WSe2 crystals by CER, PR, and PzR spectroscopy, i.e., techniques which are very sensitive to critical points of Brillouin zone. For the four crystals besides the A transition at K point, an AH transition at H point has been observed in CER, PR, and PzR spectra a few tens of meV above the A transition. The spectral difference between A and AH transition has been found to be in a very good agreement with theoretical predictions. The second transition at the H point of Brillouin zone (BH transition) overlaps spectrally with the B transition at K point because of small energy differences in the valence (conduction) band positions at H and K points. Therefore, an extra resonance which could be related to the BH transition is not resolved in modulated reflectance spectra at room temperature for the four crystals. [ABSTRACT FROM AUTHOR]

Engineering non-linear hybrid light-matter states in tailored lattices is a central research strategy for the simulation of complex Hamiltonians. Excitons in atomically thin crystals are an ideal active medium for such purposes, since they couple strongly with light and bear the potential to harness giant non-linearities and interactions while presenting a simple sample-processing and room temperature operability. We demonstrate lattice polaritons, based on an open, high-quality optical cavity, with an imprinted photonic lattice strongly coupled to excitons in a WS2 monolayer. We experimentally observe the emergence of the canonical band-structure of particles in a one-dimensional lattice at room temperature, and demonstrate frequency reconfigurability over a spectral window exceeding 85 meV, as well as the systematic variation of the nearest-neighbour coupling, reflected by a tunability in the bandwidth of the p-band polaritons by 7 meV. The technology presented in this work is a critical demonstration towards reconfigurable photonic emulators operated with non-linear photonic fluids, offering a simple experimental implementation and working at ambient conditions. Excitons in atomically thin crystals couple strongly with light. Here, the authors observe lattice polaritons in a tunable open optical cavity at room temperature, with an imprinted photonic lattice strongly coupled to excitons in a WS2 monolayer. [ABSTRACT FROM AUTHOR]

The recent discovery of magnetism in monolayers of two-dimensional van der Waals materials has opened new venues in materials science and condensed matter physics. Until recently, two-dimensional magnetism remained elusive: Spontaneous magnetic order is a routine instance in three-dimensional materials but it is not a priori guaranteed in the two-dimensional world. Since the 2016 discovery of antiferromagnetism in monolayer FePS3 by two groups and the subsequent demonstration of ferromagnetic order in monolayer CrI3 and bilayer Cr2Ge2Te6, the field changed dramatically. Within several years of scientific discoveries focused on 2D magnets, novel opportunities have opened up in the field of spintronics, namely spin pumping devices, spin transfer torque, and tunneling. In this review, we describe the state of the art of the nascent field of magnetic two-dimensional materials focusing on synthesis, engineering, and theory aspects. We also discuss challenges and some of the many different promising directions for future work, highlighting unique applications that may extend even to other realms, including sensing and data storage. [ABSTRACT FROM AUTHOR]

Two-dimensional (2D) Janus materials are a new class of materials with unique physical, chemical, and quantum properties. The name "Janus" originates from the ancient Roman god which has two faces, one looking to the future while the other facing the past. Janus has been used to describe special types of materials which have two faces at the nanoscale. This unique atomic arrangement has been shown to present rather exotic properties with applications in biology, chemistry, energy conversion, and quantum sciences. This review article aims to offer a comprehensive review of the emergent quantum properties of Janus materials. The review starts by introducing 0D Janus nanoparticles and 1D Janus nanotubes, and highlights their difference from classical ones. The design principles, synthesis, and the properties of graphene-based and chalcogenide-based Janus layers are then discussed. A particular emphasis is given to colossal built-in potential in 2D Janus layers and resulting quantum phenomena such as Rashba splitting, skyrmionics, excitonics, and 2D magnetic ordering. More recent theoretical predictions are discussed in 2D Janus superlattices when Janus layers are stacked onto each other. Finally, we discuss the tunable quantum properties and newly predicted 2D Janus layers waiting to be experimentally realized. The review serves as a complete summary of the 2D Janus library and predicted quantum properties in 2D Janus layers and their superlattices. [ABSTRACT FROM AUTHOR]

We investigate valley exciton dynamics in MoSe2 monolayers in polarization- and time-resolved photoluminescence (PL) spectroscopy at 4 K. Following circularly polarized laser excitation, we record a low circular polarization degree of the PL of typically ≤5%. This is about 10 times lower than the polarization induced under comparable conditions in MoS2 and WSe2 monolayers. The evolution of the exciton polarization as a function of excitation laser energy and power is monitored in PL excitation experiments. Fast PL emission times are recorded for both the neutral exciton of ≤3 ps and for the charged exciton (trion) of 12 ps. [ABSTRACT FROM AUTHOR]

Abstract: We provide experimental evidence for the existence of ferromagnetism in bilayers of Pd/C60 which is supported by theoretical calculations based on density functional theory (DFT). The observed ferromagnetism is surprising as C60 and Pd films are both non-ferromagnetic in the non-interacting limit. Magnetization (M) versus applied field (H) data acquired at different temperatures (T) show magnetic hysteresis with typical coercive fields (H c ) on the order of 50Oe. From the temperature-dependent magnetization M(T) we extract a Curie temperature ( ) using Bloch-like power law extrapolations to high temperatures. Using DFT calculations we investigated all plausible scenarios for the interaction between the C60 molecules and the Pd slabs, Pd single atoms and Pd clusters. DFT shows that while the C60 molecules are nonmagnetic, Pd films have a degenerate ground state that, subject to a weak perturbation, can become ferromagnetic. Calculations also show that the interaction of C60 molecules with excess Pd atoms and with sharp edges of a Pd slab is the most likely configuration that render the system ferromagnetic. Interestingly, the calculated charge transfer (0.016 e per surface Pd atom, 0.064 e per Pd for intimate contact region) between C60 and Pd does not appear to play an important role. [Copyright &y& Elsevier]

Typical Raman spectra of transition-metal dichalcogenides (TMDs) display two prominent peaks, E2g and A1g, that are well separated from each other. We find that these modes are degenerate in bulk WSe2 yielding one single Raman peak in contrast to other TMDs. As the dimensionality is lowered, the observed peak splits in two. In contrast, our ab initio calculations predict that the degeneracy is retained even for WSe2 monolayers. Interestingly, for minuscule biaxial strain, the degeneracy is preserved, but once the crystal symmetry is broken by a small uniaxial strain, the degeneracy is lifted. Our calculated phonon dispersion for uniaxially strained WSe2 shows a good match to the measured Raman spectrum, which suggests that uniaxial strain exists in WSe2 flakes, possibly induced during the sample preparation and/or as a result of the interaction between WSe2 and the substrate. Furthermore, we find that WSe2 undergoes an indirect-to-direct band-gap transition from bulk to monolayers, which is ubiquitous for semiconducting TMDs. These results not only allow us to understand the vibrational and electronic properties of WSe2, but also point to effects of the interaction between the monolayer TMDs and the substrate on the vibrational and electronic properties. [ABSTRACT FROM AUTHOR]

We describe a straightforward technique for selective graphene growth and nanoribbon production onto 4H- and 6H-SiC. The technique presented is as easy as ion implanting regions where graphene layers are desired followed by annealing to 100 °C below the graphitization temperature (TG) of SiC. We find that ion implantation of SiC lowers the TG, allowing selective graphene growth at temperatures below the TG of pristine SiC and above TG of implanted SiC. This results in an approach for patterning device structures ranging from a couple tens of nanometers to microns in size without using conventional lithography and chemical processing. [ABSTRACT FROM AUTHOR]

A thin Al2O3 insulating buffer layer deposited on indium tin oxide (ITO) anode by atomic layer deposition has been investigated for organic light-emitting diodes (OLEDs). With an optimal thickness of 1.4 nm and low density of structural defects of the Al2O3 film, the OLEDs current efficiency and power efficiency were simultaneously improved by 12.5% and 23.4%, respectively. The improvements in both current and power efficiency mean lower energy loss during holes injection process and better balanced charge injection. To understand the mechanism behind the enhanced performance of OLED by the buffer layer, a series of Al2O3 films of different thicknesses were deposited on ITO anode and characterized. The roughness, sheet resistance, and surface potential (EF′) of the Al2O3 modified ITO were characterized. Also, the properties of Al2O3 films were investigated at the device level. It is believed that the block of holes injection by the Al2O3 buffer layer makes more balanced carrier density in the emitting layer, thus enhances the current efficiency. Although less number of holes are injected into OLED due to the Al2O3 buffer layer, quantum tunneling through the ultra-thin buffer layer play an important role in contributing to the holes injection, which avoids crossing the interface barrier, resulting in less energy consumed and power efficiency enhanced. [ABSTRACT FROM AUTHOR]

Rectification and thermal stability of diodes formed at graphene/GaN interfaces have been investigated using Raman Spectroscopy and temperature-dependent current-voltage measurements. The Schottky barriers formed between GaN and mechanically transferred graphene display rectification that is preserved up to 550 K with the diodes eventually becoming non-rectifying above 650 K. Upon cooling, the diodes show excellent recovery with improved rectification. We attribute these effects to the thermal stability of graphene, which acts like an impenetrable barrier to the diffusion of contaminants across the interface, and to changes in the interface band alignment associated with thermally induced dedoping of graphene. [ABSTRACT FROM AUTHOR]

We demonstrate the formation of semimetal graphite/semiconductor Schottky barriers where the semiconductor is either silicon (Si), gallium arsenide (GaAs), or 4H-silicon carbide (4H-SiC). Near room temperature, the forward-bias diode characteristics are well described by thermionic emission, and the extracted barrier heights, which are confirmed by capacitance voltage measurements, roughly follow the Schottky–Mott relation. Since the outermost layer of the graphite electrode is a single graphene sheet, we expect that graphene/semiconductor barriers will manifest similar behavior. [ABSTRACT FROM AUTHOR]

A systematic first-principles study of atomic strings made by group IV, III–V, and II–VI elements has revealed interesting mechanical, electronic, and transport properties. The double bond structure underlies their unusual properties. We found that linear chain of C, Si, Ge, SiGe, GaAs, InSb, and CdTe are stable and good conductor, although their parent diamond (zincblende) crystals are covalent (polar) semiconductors but, compounds SiC, BN, AlP, and ZnSe are semiconductors. First row elements do not form zigzag structures. [ABSTRACT FROM AUTHOR]

Dielectric engineering of heterostructures made from two-dimensional van der Waals semiconductors is a unique and powerful tool to tailor the electric and optical band gaps solely via the dielectric environment and the crystal thickness modulation. Here, we utilize high quality MoTe2 monolayer and bilayer crystals as a candidate for near-infrared photonic applications. The crystals are exfoliated on various technologically relevant carrier substrates: silicon/silicon dioxide, poly(methyl methacrylate), hexagonal boron nitride, silicon carbide, and silicon nitride. These substrates provide a large range of high frequency dielectric constants from 2.1 to 7.0 for MoTe2-containing heterostructures. We assess the relationship between the environmental dielectric function and Coulomb screening by combining detailed spectroscopic measurements, utilizing low-temperature and high-spatially resolved photoluminescence and contrast reflectivity, with microscopic many-body modeling, to explore the potential of this less-recognized material platform for applications in optoelectronics at photon wavelengths above 1 μm. We observe a redshift of the optical gap emission energy from the monolayer to bilayer regime on the order of 30 meV. Furthermore, the thickness controlled shift is slightly larger than the one induced by the local dielectric environment, which ranges on the order of 20 meV for the MoTe2 monolayers and on the order of 8 meV for the MoTe2 bilayers. We also show that the local dielectric screening barely affects the trion binding energy, which is captured by our microscopic model, accounting for the screened Coulomb potential for the heterostructures. [ABSTRACT FROM AUTHOR]

We investigate the optical properties of bromine-intercalated highly orientated pyrolytic graphite (Br-HOPG) and provide an interpretation of the data. We observe absorption features below 620 meV which are absent in the absorption spectrum of graphite. Comparing our results with those of theoretical studies on graphite, single- and bilayer graphene, as well as recent optical studies of multilayer graphene, we conclude that Br-HOPG contains the signatures of ultrapure bilayer graphene, ultrapure single-layer graphene, and graphite. The observed supermetallic conductivity of Br-HOPG is identified with the presence of very high mobility (≃121 000 cm2V-1s-1 at room temperature and at very high carrier density), multilayer graphene components in our sample. This could provide an avenue for single- and multilayer graphene research. [ABSTRACT FROM AUTHOR]

Modulated reflectance (contactless electroreflectance (CER), photoreflectance (PR), and piezoreflectance (PzR)) has been applied to study direct optical transitions in bulk MoS2, MoSe2, WS2, and WSe2. In order to interpret optical transitions observed in CER, PR, and PzR spectra, the electronic band structure for the four crystals has been calculated from the first principles within the density functional theory for various points of Brillouin zone including K and H points. It is clearly shown that the electronic band structure at H point of Brillouin zone is very symmetric and similar to the electronic band structure at K point, and therefore, direct optical transitions at H point should be expected in modulated reflectance spectra besides the direct optical transitions at the K point of Brillouin zone. This prediction is confirmed by experimental studies of the electronic band structure of MoS2, MoSe2, WS2, and WSe2 crystals by CER, PR, and PzR spectroscopy, i.e., techniques which are very sensitive to critical points of Brillouin zone. For the four crystals besides the A transition at K point, an AH transition at H point has been observed in CER, PR, and PzR spectra a few tens of meV above the A transition. The spectral difference between A and AH transition has been found to be in a very good agreement with theoretical predictions. The second transition at the H point of Brillouin zone (BH transition) overlaps spectrally with the B transition at K point because of small energy differences in the valence (conduction) band positions at H and K points. Therefore, an extra resonance which could be related to the BH transition is not resolved in modulated reflectance spectra at room temperature for the four crystals. [ABSTRACT FROM AUTHOR]

Ca(OH)2 crystals, well known as portlandite, are grown in layered form, and we found that they can be exfoliated on different substrates. We performed first principles calculations to investigate the structural, electronic, vibrational, and mechanical properties of bulk, bilayer, and monolayer structures of this material. Different from other lamellar structures such as graphite and transition-metal dichalcogenides, intralayer bonding in Ca(OH)2 is mainly ionic, while the interlayer interaction remains a weak dispersion-type force. Unlike well-known transition-metal dichalcogenides that exhibit an indirect-to-direct band gap crossover when going from bulk to a single layer, Ca(OH)2 is a direct band gap semiconductor independent of the number layers. The in-plane Young's modulus and the in-plane shear modulus of monolayer Ca(OH)2 are predicted to be quite low while the in-plane Poisson ratio is larger in comparison to those in the monolayer of ionic crystal BN. We measured the Raman spectrum of bulk Ca(OH)2 and identified the high-frequency OH stretching mode A1g at 3620cm-1. In this study, bilayer and monolayer portlandite [Ca(OH)2] are predicted to be stable and their characteristics are analyzed in detail. Our results can guide further research on ultrathin hydroxites. [ABSTRACT FROM AUTHOR]

Recently, rhenium disulfide (ReS2) monolayers were experimentally extracted by conventional mechanical exfoliation technique from as-grown ReS2 crystals. Unlike the well-known members of transition metal dichalcogenides (TMDs), ReS2 crystallizes in a stable distorted-1T structure and lacks an indirect to direct gap crossover. Here we present an experimental and theoretical study of the formation, energetics, and stability of the most prominent lattice defects in monolayer ReS2. Experimentally, irradiation with 3-MeV He+2 ions was used to break the strong covalent bonds in ReS2 flakes. Photoluminescence measurements showed that the luminescence from monolayers is mostly unchanged after highly energetic a particle irradiation. In order to understand the energetics of possible vacancies in ReS2 we performed systematic first-principles calculations. Our calculations revealed that the formation of a single sulfur vacancy has the lowest formation energy in both Re and S rich conditions and a random distribution of such defects are energetically more preferable. Sulfur point defects do not result in any spin polarization whereas the creation of Re-containing point defects induce magnetization with a net magnetic moment of 1-3μB. Experimentally observed easy formation of sulfur vacancies is in good agreement with first-principles calculations. [ABSTRACT FROM AUTHOR]

We have investigated the exciton dynamics in transition metal dichalcogenide monolayers using time-resolved photoluminescence experiments performed with optimized time resolution. For MoSe2 monolayer, we measure τrad0 = 1.8 ± 0.2 ps at T = 7K that we interpret as the intrinsic radiative recombination time. Similar values are found for WSe2 monolayers. Our detailed analysis suggests the following scenario: at low temperature (T ≤ 50K), the exciton oscillator strength is so large that the entire light can be emitted before the time required for the establishment of a thermalized exciton distribution. For higher lattice temperatures, the photoluminescence dynamics is characterized by two regimes with very different characteristic times. First the photoluminescence intensity drops drastically with a decay time in the range of the picosecond driven by the escape of excitons from the radiative window due to exciton-phonon interactions. Following this first nonthermal regime, a thermalized exciton population is established gradually yielding longer photoluminescence decay times in the nanosecond range. Both the exciton effective radiative recombination and nonradiative recombination channels including exciton-exciton annihilation control the latter. Finally the temperature dependence of the measured exciton and trion dynamics indicates that the two populations are not in thermodynamical equilibrium. [ABSTRACT FROM AUTHOR]

Moiré superlattices of semiconducting transition metal dichalcogenide heterobilayers are model systems for investigating strongly correlated electronic phenomena. Specifically, WSe 2 /WS 2 moiré superlattices have emerged as a quantum simulator for the two-dimensional extended Hubbard model. Experimental studies of charge transport have revealed correlated Mott insulator and generalized Wigner crystal states, but spin transport of the moiré heterostructure has not yet been sufficiently explored. Here, we use spatially and temporally resolved circular dichroism spectroscopy to directly image the spin transport as a function of carrier doping and temperature in WSe 2 /WS 2 moiré heterostructures. We observe diffusive spin transport at all hole concentrations at 11 Kelvin - including the Mott insulator at one hole per moiré unit cell - where charge transport is strongly suppressed. At elevated temperatures the spin diffusion constant remains unchanged in the Mott insulator state, but it increases significantly at finite doping away from the Mott state. The doping- and temperature-dependent spin transport can be qualitatively understood using a t-J model, where spins can move via the hopping of spin-carrying charges and via the exchange interaction., Competing Interests: Competing interests: The authors declare no competing interests., (© 2024. The Author(s).)

Semiconductor moiré superlattices provide a versatile platform to engineer quantum solids composed of artificial atoms on moiré sites. Previous studies have mostly focused on the simplest correlated quantum solid-the Fermi-Hubbard model-in which intra-atom interactions are simplified to a single onsite repulsion energy U . Here we report the experimental observation of Wigner molecular crystals emerging from multielectron artificial atoms in twisted bilayer tungsten disulfide moiré superlattices. Using scanning tunneling microscopy, we demonstrate that Wigner molecules appear in multielectron artificial atoms when Coulomb interactions dominate. The array of Wigner molecules observed in a moiré superlattice comprises a crystalline phase of electrons: the Wigner molecular crystal, which is shown to be highly tunable through mechanical strain, moiré period, and carrier charge type.

One-dimensional (1D) interacting electrons are often described as a Luttinger liquid 1-4 having properties that are intrinsically different from those of Fermi liquids in higher dimensions 5,6 . In materials systems, 1D electrons exhibit exotic quantum phenomena that can be tuned by both intra- and inter-1D-chain electronic interactions, but their experimental characterization can be challenging. Here we demonstrate that layer-stacking domain walls (DWs) in van der Waals heterostructures form a broadly tunable Luttinger liquid system, including both isolated and coupled arrays. We have imaged the evolution of DW Luttinger liquids under different interaction regimes tuned by electron density using scanning tunnelling microscopy. Single DWs at low carrier density are highly susceptible to Wigner crystallization consistent with a spin-incoherent Luttinger liquid, whereas at intermediate densities dimerized Wigner crystals form because of an enhanced magneto-elastic coupling. Periodic arrays of DWs exhibit an interplay between intra- and inter-chain interactions that gives rise to new quantum phases. At low electron densities, inter-chain interactions are dominant and induce a 2D electron crystal composed of phased-locked 1D Wigner crystal in a staggered configuration. Increased electron density causes intra-chain fluctuation potentials to dominate, leading to an electronic smectic liquid crystal phase in which electrons are ordered with algebraical correlation decay along the chain direction but disordered between chains. Our work shows that layer-stacking DWs in 2D heterostructures provides opportunities to explore Luttinger liquid physics., (© 2024. The Author(s), under exclusive licence to Springer Nature Limited.)

Moiré superlattices provide a highly tuneable and versatile platform to explore novel quantum phases and exotic excited states ranging from correlated insulators to moiré excitons. Scanning tunnelling microscopy has played a key role in probing microscopic behaviours of the moiré correlated ground states at the atomic scale. However, imaging of quantum excited states in moiré heterostructures remains an outstanding challenge. Here we develop a photocurrent tunnelling microscopy technique that combines laser excitation and scanning tunnelling spectroscopy to directly visualize the electron and hole distribution within the photoexcited moiré exciton in twisted bilayer WS 2 . The tunnelling photocurrent alternates between positive and negative polarities at different locations within a single moiré unit cell. This alternating photocurrent originates from the in-plane charge transfer moiré exciton in twisted bilayer WS 2 , predicted by our GW-Bethe-Salpeter equation calculations, that emerges from the competition between the electron-hole Coulomb interaction and the moiré potential landscape. Our technique enables the exploration of photoexcited non-equilibrium moiré phenomena at the atomic scale., (© 2024. The Author(s), under exclusive licence to Springer Nature Limited.)

Transition metal dichalcogenide-based moiré superlattices exhibit strong electron-electron correlations, thus giving rise to strongly correlated quantum phenomena such as generalized Wigner crystal states. Evidence of Wigner crystals in transition metal dichalcogenide moire superlattices has been widely reported from various optical spectroscopy and electrical conductivity measurements, while their microscopic nature has been limited to the basic lattice structure. Theoretical studies predict that unusual quasiparticle excitations across the correlated gap between upper and lower Hubbard bands can arise due to long-range Coulomb interactions in generalized Wigner crystal states. However, the microscopic proof of such quasiparticle excitations is challenging because of the low excitation energy of the Wigner crystal. Here we describe a scanning single-electron charging spectroscopy technique with nanometre spatial resolution and single-electron charge resolution that enables us to directly image electron and hole wavefunctions and to determine the thermodynamic gap of generalized Wigner crystal states in twisted WS 2 moiré heterostructures. High-resolution scanning single-electron charging spectroscopy combines scanning tunnelling microscopy with a monolayer graphene sensing layer, thus enabling the generation of individual electron and hole quasiparticles in generalized Wigner crystals. We show that electron and hole quasiparticles have complementary wavefunction distributions and that thermodynamic gaps of ∼50 meV exist for the 1/3 and 2/3 generalized Wigner crystal states in twisted WS 2 ., (© 2024. The Author(s), under exclusive licence to Springer Nature Limited.)

Nitrogen doped lutetium hydride has drawn global attention in the pursuit of room-temperature superconductivity near ambient pressure and temperature. However, variable synthesis techniques and uncertainty surrounding nitrogen concentration have contributed to extensive debate within the scientific community about this material and its properties. We used a solid-state approach to synthesize nitrogen doped lutetium hydride at high pressure and temperature (HPT) and analyzed the residual starting materials to determine its nitrogen content. High temperature oxide melt solution calorimetry determined the formation enthalpy of LuH 1.96 N 0.02 (LHN) from LuH 2 and LuN to be -28.4 ± 11.4 kJ/mol. Magnetic measurements indicated diamagnetism which increased with nitrogen content. Ambient pressure conductivity measurements observed metallic behavior from 5 to 350 K, and the constant and parabolic magnetoresistance changed with increasing temperature. High pressure conductivity measurements revealed that LHN does not exhibit superconductivity up to 26.6 GPa. We compressed LHN in a diamond anvil cell to 13.7 GPa and measured the Raman signal at each step, with no evidence of any phase transition. Despite the absence of superconductivity, a color change from blue to purple to red was observed with increasing pressure. Thus, our findings confirm the thermodynamic stability of LHN, do not support superconductivity, and provide insights into the origins of its diamagnetism., Competing Interests: Competing interests statement:The authors declare no competing interest.

The ultrafast carrier dynamics of junctions between two chemically identical, but electronically distinct, transition metal dichalcogenides (TMDs) remains largely unknown. Here, we employ time-resolved photoemission electron microscopy (TR-PEEM) to probe the ultrafast carrier dynamics of a monolayer-to-multilayer (1L-ML) WSe 2 junction. The TR-PEEM signals recorded for the individual components of the junction reveal the sub-ps carrier cooling dynamics of 1L- and 7L-WSe 2 , as well as few-ps exciton-exciton annihilation occurring on 1L-WSe 2 . We observe ultrafast interfacial hole (h) transfer from 1L- to 7L-WSe 2 on an ∼0.2 ps time scale. The resultant excess h density in 7L-WSe 2 decays by carrier recombination across the junction interface on an ∼100 ps time scale. Reminiscent of the behavior at a depletion region, the TR-PEEM image reveals the h density accumulation on the 7L-WSe 2 interface, with a decay length ∼0.60 ± 0.17 μm. These charge transfer and recombination dynamics are in agreement with ab initio quantum dynamics. The computed orbital densities reveal that charge transfer occurs from the basal plane, which extends over both 1L and ML regions, to the upper plane localized on the ML region. This mode of charge transfer is distinctive to chemically homogeneous junctions of layered materials and constitutes an additional carrier deactivation pathway that should be considered in studies of 1L-TMDs found alongside their ML, a common occurrence in exfoliated samples.

Coupled two-dimensional electron-hole bilayers provide a unique platform to study strongly correlated Bose-Fermi mixtures in condensed matter. Electrons and holes in spatially separated layers can bind to form interlayer excitons, composite Bosons expected to support high-temperature exciton condensates. The interlayer excitons can also interact strongly with excess charge carriers when electron and hole densities are unequal. Here, we use optical spectroscopy to quantitatively probe the local thermodynamic properties of strongly correlated electron-hole fluids in MoSe 2 /hBN/WSe 2 heterostructures. We observe a discontinuity in the electron and hole chemical potentials at matched electron and hole densities, a definitive signature of an excitonic insulator ground state. The excitonic insulator is stable up to a Mott density of ~0.8 × 10 12 cm -2 and has a thermal ionization temperature of ~70 K. The density dependence of the electron, hole, and exciton chemical potentials reveals strong correlation effects across the phase diagram. Compared with a non-interacting uniform charge distribution, the correlation effects lead to significant attractive exciton-exciton and exciton-charge interactions in the electron-hole fluid. Our work highlights the unique quantum behavior that can emerge in strongly correlated electron-hole systems., (© 2023. The Author(s).)

Bosonic condensation and lasing of exciton polaritons in microcavities is a fascinating solid-state phenomenon. It provides a versatile platform to study out-of-equilibrium many-body physics and has recently appeared at the forefront of quantum technologies. Here, we study the photon statistics via the second-order temporal correlation function of polariton lasing emerging from an optical microcavity with an embedded atomically thin MoSe_{2} crystal. Furthermore, we investigate the macroscopic polariton phase transition for varying excitation powers and temperatures. The lower-polariton exhibits photon bunching below the threshold, implying a dominant thermal distribution of the emission, while above the threshold, the second-order correlation transits towards unity, which evidences the formation of a coherent state. Our findings are in agreement with a microscopic numerical model, which explicitly includes scattering with phonons on the quantum level.

Solid-state single-photon sources are central building blocks in quantum information processing. Atomically thin crystals have emerged as sources of nonclassical light; however, they perform below the state-of-the-art devices based on volume crystals. Here, we implement a bright single-photon source based on an atomically thin sheet of WSe 2 coupled to a tunable optical cavity in a liquid-helium-free cryostat without the further need for active stabilization. Its performance is characterized by high single-photon purity (g (2) (0) = 4.7 ± 0.7%) and record-high, first-lens brightness of linearly polarized photons of 65 ± 4%, representing a decisive step toward real-world quantum applications. The high performance of our devices allows us to observe two-photon interference in a Hong-Ou-Mandel experiment with 2% visibility limited by the emitter coherence time and setup resolution. Our results thus demonstrate that the combination of the unique properties of two-dimensional materials and versatile open cavities emerges as an inspiring avenue for novel quantum optoelectronic devices.

Strain engineering is an attractive approach for tuning the local optoelectronic properties of transition metal dichalcogenides (TMDs). While strain has been shown to affect the nanosecond carrier recombination dynamics of TMDs, its influence on the sub-picosecond electronic relaxation dynamics is still unexplored. Here, we employ a combination of time-resolved photoemission electron microscopy (TR-PEEM) and nonadiabatic ab initio molecular dynamics (NAMD) to investigate the ultrafast dynamics of wrinkled multilayer (ML) MoS 2 comprising 17 layers. Following 2.41 eV photoexcitation, electronic relaxation at the Γ valley occurs with a time constant of 97 ± 2 fs for wrinkled ML-MoS 2 and 120 ± 2 fs for flat ML-MoS 2 . NAMD shows that wrinkling permits larger amplitude motions of MoS 2 layers, relaxes electron-phonon coupling selection rules, perturbs chemical bonding, and increases the electronic density of states. As a result, the nonadiabatic coupling grows and electronic relaxation becomes faster compared to flat ML-MoS 2 . Our study suggests that the sub-picosecond electronic relaxation dynamics of TMDs is amenable to strain engineering and that applications which require long-lived hot carriers, such as hot-electron-driven light harvesting and photocatalysis, should employ wrinkle-free TMDs.

Moiré superlattices of semiconducting transition metal dichalcogenides enable unprecedented spatial control of electron wavefunctions, leading to emerging quantum states. The breaking of translational symmetry further introduces a new degree of freedom: high symmetry moiré sites of energy minima behaving as spatially separated quantum dots. We demonstrate the superposition between two moiré sites by constructing a trilayer WSe 2 /monolayer WS 2 moiré heterojunction. The two moiré sites in the first layer WSe 2 interfacing WS 2 allow the formation of two different interlayer excitons, with the hole residing in either moiré site of the first layer WSe 2 and the electron in the third layer WSe 2 . An electric field can drive the hybridization of either of the interlayer excitons with the intralayer excitons in the third WSe 2 layer, realizing the continuous tuning of interlayer exciton hopping between two moiré sites and a superposition of the two interlayer excitons, distinctively different from the natural trilayer WSe 2 ., (© 2023. Springer Nature Limited.)

Transition metal dichalcogenide (TMDC) moiré superlattices, owing to the moiré 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 WSe 2 -WS 2 -WSe 2 trilayer moiré 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 WSe 2 valence moiré flatbands. The same mechanism also gives rise to an interlayer Mott insulator state, in which the two WSe 2 layers share one hole laterally confined in one moiré 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 WSe 2 under a large electric field, accompanying the transition from quadrupolar excitons to dipolar excitons. Our work demonstrates a trilayer moiré system as a new exciting playground for realizing novel correlated states and engineering quantum phase transitions., (© 2023. The Author(s).)

Moiré heterobilayers host interlayer excitons in a natural, periodic array of trapping potentials. Recent work has elucidated the structure of the trapped interlayer excitons and the nature of photoluminescence (PL) from trapped and itinerant charged complexes such as interlayer trions in these structures. In this paper, our results serve to add to the understanding of the nature of PL emission and explain its characteristic blueshift with increasing carrier density, along with demonstrating a significant difference between the interlayer exciton-trion conversion efficiency as compared to both localized and itinerant intralayer species in conventional monolayers. Our results show the absence of optical generation of trions in these materials, which we suggest arises from the highly localized, near subnanometer confinement of trapped species in these Moiré potentials.

van der Waals heterostructures (vdW-HSs) integrate dissimilar materials to form complex devices. These rely on the manipulation of charges at multiple interfaces. However, at present, submicrometer variations in strain, doping, or electrical breakages may exist undetected within a device, adversely affecting macroscale performance. Here, we use conductive mode and cathodoluminescence scanning electron microscopy (CM-SEM and SEM-CL) to investigate these phenomena. As a model system, we use a monolayer WSe 2 (1L-WSe 2 ) encapsulated in hexagonal boron nitride (hBN). CM-SEM allows for quantification of the flow of electrons during the SEM measurements. During electron irradiation at 5 keV, up to 70% of beam electrons are deposited into the vdW-HS and can subsequently migrate to the 1L-WSe 2 . This accumulation of charge leads to dynamic doping of 1L-WSe 2 , reducing its CL efficiency by up to 30% over 30 s. By providing a path for excess electrons to leave the sample, near full restoration of the initial CL signal can be achieved. These results indicate that the trapping of charges in vdW-HSs during electron irradiation must be considered, in order to obtain and maintain optimal performance of vdW-HS devices during processes such as e-beam lithography or SEM. Thus, CM-SEM and SEM-CL form a toolkit through which nanoscale characterization of vdW-HS devices can be performed, allowing electrical and optical properties to be correlated.