Columnar excitation fluorescence microscope for accurate evaluation of quantum properties of color centers in bulk materials.

Color centers in wide band-gap semiconductors, which have superior quantum properties even at room temperature and atmospheric pressure, have been actively applied to quantum sensing devices. Characterizing the quantum properties of the color centers in the semiconductor materials and ensuring that these properties are uniform over a wide area are key issues for developing quantum sensing devices based on color centers. In this article, we have developed an optics design protocol optimized for evaluating the quantum properties of color centers and have used this design approach to develop a new microscopy system called columnar excitation fluorescence microscope (CEFM). The essence of this system is to maximize the amount of fluorescence detection of polarized color centers, which is achieved by large-volume and uniform laser excitation along the sample thickness with sufficient laser power density. This laser excitation technique prevents undesirable transitions to undesirable charge states and undesirable light, such as unpolarized color center fluorescence, while significantly increasing the color center fluorescence. This feature enables fast measurements with a high signal-to-noise ratio, making it possible to evaluate the spatial distribution of quantum properties across an entire mm-size sample without using a darkroom, which is difficult with typical confocal microscope systems.

Metasurface of Strongly Coupled Excitons and Nanoplasmonic Arrays.

Metasurfaces allow light to be manipulated at the nanoscale. Integrating metasurfaces with transition metal dichalcogenide monolayers provides additional functionality to ultrathin optics, including tunable optical properties with enhanced light-matter interactions. In this work, we demonstrate the realization of a polaritonic metasurface utilizing the sizable light-matter coupling of excitons in monolayer WSe2 and the collective lattice resonances of nanoplasmonic gold arrays. We developed a novel fabrication method to integrate gold nanodisk arrays in hexagonal boron nitride and thus simultaneously ensure spectrally narrow exciton transitions and their immediate proximity to the near-field of array surface lattice resonances. In the regime of strong light-matter coupling, the resulting van der Waals metasurface exhibits all key characteristics of lattice polaritons, with a directional and linearly polarized far-field emission profile dictated by the underlying nanoplasmonic lattice. Our work can be straightforwardly adapted to other lattice geometries, establishing structured van der Waals metasurfaces as means to engineer polaritonic lattices.

Epitaxial growth of quasi-2D van der Waals ferromagnets on crystalline substrates.

Intrinsic magnetism in van der Waals materials has instigated interest in exploring magnetism in the 2D limit for potential applications in spintronics and also understanding of novel control of 2D magnetism by variation of layer thickness, gate tunability and magnetoelectric effects. The chromium telluride (CrxTey) family is an interesting subsection of ferromagnetic materials with high TC values, also presenting diverse stoichiometry arising from self-intercalation of Cr. Apart from the layered CrTe2 system, the other non-layered CrxTey compounds also offer exceptional magnetic properties and a novel growth technique to grow thin films of these non-layered compounds offer exciting possibilities for ultrathin spin-based electronics and magnetic sensors. In this work we have discussed the role of crystalline substrates in CVD growth of non-layered 2D ferromagnets, where the crystal symmetry of the substrate as well as the misfit and strain are the key players governing the growth mechanism of ultrathin Cr5Te8, a non-layered ferromagnet. The magnetic studies of the as-grown Cr5Te8 revealed signatures of co-existing soft and hard ferromagnetic phases which makes this system an intriguing system to search for emergent topological phases such as magnetic skyrmions.

Photocurrent Spectroscopy of Dark Magnetic Excitons in 2D Multiferroic NiI2.

Two-dimensional (2D) antiferromagnetic (AFM) semiconductors are promising components of opto-spintronic devices due to terahertz operation frequencies and minimal interactions with stray fields. However, the lack of net magnetization significantly limits the number of experimental techniques available to study the relationship between magnetic order and semiconducting properties. Here, they demonstrate conditions under which photocurrent spectroscopy can be employed to study many-body magnetic excitons in the 2D AFM semiconductor NiI2. The use of photocurrent spectroscopy enables the detection of optically dark magnetic excitons down to bilayer thickness, revealing a high degree of linear polarization that is coupled to the underlying helical AFM order of NiI2. In addition to probing the coupling between magnetic order and dark excitons, this work provides strong evidence for the multiferroicity of NiI2 down to bilayer thickness, thus demonstrating the utility of photocurrent spectroscopy for revealing subtle opto-spintronic phenomena in the atomically thin limit.

Electrically tunable layer-hybridized trions in doped WSe2 bilayers.

Doped van der Waals heterostructures host layer-hybridized trions, i.e. charged excitons with layer-delocalized constituents holding promise for highly controllable optoelectronics. Combining a microscopic theory with photoluminescence (PL) experiments, we demonstrate the electrical tunability of the trion energy landscape in naturally stacked WSe2 bilayers. We show that an out-of-plane electric field modifies the energetic ordering of the lowest lying trion states, which consist of layer-hybridized Λ -point electrons and layer-localized K-point holes. At small fields, intralayer-like trions yield distinct PL signatures in opposite doping regimes characterized by weak Stark shifts in both cases. Above a doping-asymmetric critical field, interlayer-like species are energetically favored and produce PL peaks with a pronounced Stark red-shift and a counter-intuitively large intensity arising from efficient phonon-assisted recombination. Our work presents an important step forward in the microscopic understanding of layer-hybridized trions in van der Waals heterostructures and paves the way towards optoelectronic applications based on electrically controllable atomically-thin semiconductors.

Controlled interlayer exciton ionization in an electrostatic trap in atomically thin heterostructures.

Atomically thin semiconductor heterostructures provide a two-dimensional (2D) device platform for creating high densities of cold, controllable excitons. Interlayer excitons (IEs), bound electrons and holes localized to separate 2D quantum well layers, have permanent out-of-plane dipole moments and long lifetimes, allowing their spatial distribution to be tuned on demand. Here, we employ electrostatic gates to trap IEs and control their density. By electrically modulating the IE Stark shift, electron-hole pair concentrations above 2 × 1012 cm-2 can be achieved. At this high IE density, we observe an exponentially increasing linewidth broadening indicative of an IE ionization transition, independent of the trap depth. This runaway threshold remains constant at low temperatures, but increases above 20 K, consistent with the quantum dissociation of a degenerate IE gas. Our demonstration of the IE ionization in a tunable electrostatic trap represents an important step towards the realization of dipolar exciton condensates in solid-state optoelectronic devices.

Robust Field-Free Switching Using Large Unconventional Spin-Orbit Torque in an All-Van der Waals Heterostructure.

The emerging all-van der Waals (vdW) magnetic heterostructure provides a new platform to control the magnetization by the electric field beyond the traditional spintronics devices. One promising strategy is using unconventional spin-orbit torque (SOT) exerted by the out-of-plane polarized spin current to enable deterministic magnetization switching and enhance the switching efficiency. However, in all-vdW heterostructures, large unconventional SOT remains elusive and the robustness of the field-free switching against external magnetic field has not been examined, which hinders further applications. Here, the study demonstrates the field-free switching in an all-vdW heterostructure combining a type-II Weyl semimetal TaIrTe4 and above-room-temperature ferromagnet Fe3GaTe2. The fully field-free switching can be achieved at 2.56 × 1010 A m-2 at 300 K and a large SOT effective field efficiency of the out-of-plane polarized spin current generated by TaIrTe4 is determined to be 0.37. Moreover, it is found that the switching polarity cannot be changed until the external in-plane magnetic field reaches 252 mT, indicating a robust switching against the magnetic field. The numerical simulation suggests the large unconventional SOT reduces the switching current density and enhances the robustness of the switching. The work shows that all-vdW heterostructures are promising candidates for future highly efficient and stable SOT-based devices.

Electrical switching of spin-polarized light-emitting diodes based on a 2D CrI3/hBN/WSe2 heterostructure.

Spin-polarized light-emitting diodes (spin-LEDs) convert the electronic spin information to photon circular polarization, offering potential applications including spin amplification, optical communications, and advanced imaging. The conventional control of the emitted light's circular polarization requires a change in the external magnetic field, limiting the operation conditions of spin-LEDs. Here, we demonstrate an atomically thin spin-LED device based on a heterostructure of a monolayer WSe2 and a few-layer antiferromagnetic CrI3, separated by a thin hBN tunneling barrier. The CrI3 and hBN layers polarize the spin of the injected carriers into the WSe2. With the valley optical selection rule in the monolayer WSe2, the electroluminescence exhibits a high degree of circular polarization that follows the CrI3 magnetic states. Importantly, we show an efficient electrical tuning, including a sign reversal, of the electroluminescent circular polarization by applying an electrostatic field due to the electrical tunability of the few-layer CrI3 magnetization. Our results establish a platform to achieve on-demand operation of nanoscale spin-LED and electrical control of helicity for device applications.

Strongly coupled edge states in a graphene quantum Hall interferometer.

Electronic interferometers using the chiral, one-dimensional (1D) edge channels of the quantum Hall effect (QHE) can demonstrate a wealth of fundamental phenomena. The recent observation of phase jumps in a Fabry-Pérot (FP) interferometer revealed anyonic quasiparticle exchange statistics in the fractional QHE. When multiple integer edge channels are involved, FP interferometers have exhibited anomalous Aharonov-Bohm (AB) interference frequency doubling, suggesting putative pairing of electrons into 2 e quasiparticles. Here, we use a highly tunable graphene-based QHE FP interferometer to observe the connection between interference phase jumps and AB frequency doubling, unveiling how strong repulsive interaction between edge channels leads to the apparent pairing phenomena. By tuning electron density in-situ from filling factor ν < 2 to ν > 7 , we tune the interaction strength and observe periodic interference phase jumps leading to AB frequency doubling. Our observations demonstrate that the combination of repulsive interaction between the spin-split ν = 2 edge channels and charge quantization is sufficient to explain the frequency doubling, through a near-perfect charge screening between the localized and extended edge channels. Our results show that interferometers are sensitive probes of microscopic interactions and enable future experiments studying correlated electrons in 1D channels using density-tunable graphene.

Direct Visualization of Defect-Controlled Diffusion in van der Waals Gaps.

Diffusion processes govern fundamental phenomena such as phase transformations, doping, and intercalation in van der Waals (vdW) bonded materials. Here, the diffusion dynamics of W atoms by visualizing the motion of individual atoms at three different vdW interfaces: hexagonal boron nitride (BN)/vacuum, BN/BN, and BN/WSe2, by recording scanning transmission electron microscopy movies is quantified. Supported by density functional theory (DFT) calculations, it is inferred that in all cases diffusion is governed by intermittent trapping at electron beam-generated defect sites. This leads to diffusion properties that depend strongly on the number of defects. These results suggest that diffusion and intercalation processes in vdW materials are highly tunable and sensitive to crystal quality. The demonstration of imaging, with high spatial and temporal resolution, of layers and individual atoms inside vdW heterostructures offers possibilities for direct visualization of diffusion and atomic interactions, as well as for experiments exploring atomic structures, their in situ modification, and electrical property measurements of active devices combined with atomic resolution imaging.

In situ via Contact to hBN-Encapsulated Air-Sensitive Atomically Thin Semiconductors.

Establishing reliable electrical contacts to atomically thin materials is a prerequisite for both fundamental studies and applications yet remains a challenge. In particular, the development of contact techniques for air-sensitive monolayers has lagged behind, despite their unique properties and significant potential for applications. Here, we present a robust method to create contacts to device layers encapsulated within hexagonal boron nitride (hBN). This method uses plasma etching and metal deposition to create 'vias' in the hBN with graphene forming an atomically thin etch-stop. The resulting partially fluorinated graphene (PFG) protects the underlying device layer from air-induced degradation and damage during metal deposition. PFG is resistive in-plane but maintains high out-of-plane conductivity. The work function of the PFG/metal contact is tunable through the degree of fluorination, offering opportunities for contact engineering. Using the in situ via technique, we achieve ambipolar contact to air-sensitive monolayer 2H-molybdenum ditelluride (MoTe2) with more than 1 order of magnitude improvement in on-current density compared to previous literature. The complete encapsulation provides high reproducibility and long-term stability. The technique can be extended to other air-sensitive materials as well as air-stable materials, offering highly competitive device performance.

Sliding Memristor in Parallel-Stacked Hexagonal Boron Nitride.

Sliding ferroelectricity in 2D materials, arising from interlayer sliding-induced interlayer hybridization and charge redistribution at the van der Waals interface, offers a means to manipulate spontaneous polarization at the atomic scale through various methods such as stacking order, interfacial contact, and electric field. However, the practical application of extending 2D sliding ferroelectricity remains challenging due to the contentious mechanisms and the complex device structures required for ferroelectric switching. Here, a sliding memristor based on a graphene/parallel-stacked hexagonal boron nitride/graphene tunneling device, featuring a stable memristive hysteresis induced by interfacial polarizations and barrier height modulations, is presented. As the tunneling current density increases, the memristive window broadens, achieving an on/off ratio of ≈103 and 2 order decrease of the trigger current density, attributed to the interlayer migration of positively charged boron ions and the formation of conductive filaments, as supported by the theoretical calculations. The findings open a path for exploring the sliding memristor via a tunneling device and bridge the gap between sliding ferroelectricity and memory applications.

Wigner molecular crystals from multielectron moiré artificial atoms.

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.

Electroluminescence from pure resonant states in hBN-based vertical tunneling junctions.

Defect centers in wide-band-gap crystals have garnered interest for their potential in applications among optoelectronic and sensor technologies. However, defects embedded in highly insulating crystals, like diamond, silicon carbide, or aluminum oxide, have been notoriously difficult to excite electrically due to their large internal resistance. To address this challenge, we realized a new paradigm of exciting defects in vertical tunneling junctions based on carbon centers in hexagonal boron nitride (hBN). The rational design of the devices via van der Waals technology enabled us to raise and control optical processes related to defect-to-band and intradefect electroluminescence. The fundamental understanding of the tunneling events was based on the transfer of the electronic wave function amplitude between resonant defect states in hBN to the metallic state in graphene, which leads to dramatic changes in the characteristics of electrons due to different band structures of constituent materials. In our devices, the decay of electrons via tunneling pathways competed with radiative recombination, resulting in an unprecedented degree of tuneability of carrier dynamics due to the significant sensitivity of the characteristic tunneling times on the thickness and structure of the barrier. This enabled us to achieve a high-efficiency electrical excitation of intradefect transitions, exceeding by several orders of magnitude the efficiency of optical excitation in the sub-band-gap regime. This work represents a significant advancement towards a universal and scalable platform for electrically driven devices utilizing defect centers in wide-band-gap crystals with properties modulated via activation of different tunneling mechanisms at a level of device engineering.

Anomalous Interlayer Exciton Diffusion in WS2/WSe2 Moiré Heterostructure.

Stacking van der Waals crystals allows for the on-demand creation of a periodic potential landscape to tailor the transport of quasiparticle excitations. We investigate the diffusion of photoexcited electron-hole pairs, or excitons, at the interface of WS2/WSe2 van der Waals heterostructure over a wide range of temperatures. We observe the appearance of distinct interlayer excitons for parallel and antiparallel stacking and track their diffusion through spatially and temporally resolved photoluminescence spectroscopy from 30 to 250 K. While the measured exciton diffusivity decreases with temperature, it surprisingly plateaus below 90 K. Our observations cannot be explained by classical models like hopping in the moiré potential. A combination of ab initio theory and molecular dynamics simulations suggests that low-energy phonons arising from the mismatched lattices of moiré heterostructures, also known as phasons, play a key role in describing and understanding this anomalous behavior of exciton diffusion. Our observations indicate that the moiré potential landscape is dynamic down to very low temperatures and that the phason modes can enable efficient transport of energy in the form of excitons.

Imaging tunable Luttinger liquid systems in van der Waals heterostructures.

One-dimensional (1D) interacting electrons are often described as a Luttinger liquid1-4 having properties that are intrinsically different from those of Fermi liquids in higher dimensions5,6. 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.

Tunable even- and odd-denominator fractional quantum Hall states in trilayer graphene.

Fractional quantum Hall (FQH) states are exotic quantum many-body phases whose elementary charged excitations are anyons obeying fractional braiding statistics. While most FQH states are believed to have Abelian anyons, the Moore-Read type states with even denominators - appearing at half filling of a Landau level (LL) - are predicted to possess non-Abelian excitations with appealing potential in topological quantum computation. These states, however, depend sensitively on the orbital contents of the single-particle LL wavefunctions and the LL mixing. Here we report magnetotransport measurements on Bernal-stacked trilayer graphene, whose multiband structure facilitates interlaced LL mixing, which can be controlled by external magnetic and displacement fields. We observe robust FQH states including even-denominator ones at filling factors ν = - 9/2, - 3/2, 3/2 and 9/2. In addition, we fine-tune the LL mixing and crossings to drive quantum phase transitions of these half-filling states and neighbouring odd-denominator ones, exhibiting related emerging and waning behaviour.

Tuning Exciton Emission via Ferroelectric Polarization at a Heterogeneous Interface between a Monolayer Transition Metal Dichalcogenide and a Perovskite Oxide Membrane.

We demonstrate the integration of a thin BaTiO3 (BTO) membrane with monolayer MoSe2 in a dual-gate device that enables in situ manipulation of the BTO ferroelectric polarization with a voltage pulse. While two-dimensional (2D) transition metal dichalcogenides (TMDs) offer remarkable adaptability, their hybrid integration with other families of functional materials beyond the realm of 2D materials has been challenging. Released functional oxide membranes offer a solution for 2D/3D integration via stacking. 2D TMD excitons can serve as a local probe of the ferroelectric polarization in BTO at a heterogeneous interface. Using photoluminescence (PL) of MoSe2 excitons to optically read out the doping level, we find that the relative population of charge carriers in MoSe2 depends sensitively on the ferroelectric polarization. This finding points to a promising avenue for future-generation versatile sensing devices with high sensitivity, fast readout, and diverse applicability for advanced signal processing.

Correlated Charge Density Wave Insulators in Chirally Twisted Triple Bilayer Graphene.

Electrons residing in a flat-band system can play a vital role in triggering spectacular phenomenology due to relatively large interactions and spontaneous breaking of different degeneracies. In this work, we demonstrate chirally twisted triple bilayer graphene, a new moiré structure formed by three pieces of helically stacked Bernal bilayer graphene, as a highly tunable flat-band system. In addition to the correlated insulators showing at integer moiré fillings, commonly attributed to interaction induced symmetry broken isospin flavors in graphene, we observe abundant insulating states at half-integer moiré fillings, suggesting a longer-range interaction and the formation of charge density wave insulators which spontaneously break the moiré translation symmetry. With weak out-of-plane magnetic field applied, as observed half-integer filling states are enhanced and more quarter-integer filling states appear, pointing toward further quadrupling moiré unit cells. The insulating states at fractional fillings combined with Hartree-Fock calculations demonstrate the observation of a new type of correlated charge density wave insulators in graphene and points to a new accessible twist manner engineering correlated moiré electronics.

Magneto-Thermoelectric Transport in Graphene Quantum Dot with Strong Correlations.

Disorder at etched edges of graphene quantum dots (GQD) enables random all-to-all interactions between localized charges in partially filled Landau levels, providing a potential platform to realize the Sachdev-Ye-Kitaev (SYK) model. We use quantum Hall edge states in the graphene electrodes to measure electrical conductance and thermoelectric power across the GQD. In specific temperature ranges, we observe a suppression of electric conductance fluctuations and slowly decreasing thermoelectric power across the GQD with increasing temperature, consistent with recent theory for the SYK regime.