Electroluminescent vertical tunneling junctions based on WSe2 monolayer quantum emitter arrays: Exploring tunability with electric and magnetic fields.

We experimentally demonstrate the creation of defects in monolayer WSe2 via nanopillar imprinting and helium ion irradiation. Based on the first method, we realize atomically thin vertical tunneling light-emitting diodes based on WSe2 monolayers hosting quantum emitters at deterministically specified locations. We characterize these emitters by investigating the evolution of their emission spectra in external electric and magnetic fields, as well as by inducing electroluminescence at low temperatures. We identify qualitatively different types of quantum emitters and classify them according to the dominant electron-hole recombination paths, determined by the mechanisms of intervalley mixing occurring in fundamental conduction and/or valence subbands.

Dielectric Environment Sensitivity of Carbon Centers in Hexagonal Boron Nitride.

A key advantage of utilizing van-der-Waals (vdW) materials as defect-hosting platforms for quantum applications is the controllable proximity of the defect to the surface or the substrate allowing for improved light extraction, enhanced coupling with photonic elements, or more sensitive metrology. However, this aspect results in a significant challenge for defect identification and characterization, as the defect's properties depend on the the atomic environment. This study explores how the environment can influence the properties of carbon impurity centers in hexagonal boron nitride (hBN). It compares the optical and electronic properties of such defects between bulk-like and few-layer films, showing alteration of the zero-phonon line energies and their phonon sidebands, and enhancements of inhomogeneous broadenings. To disentangle the mechanisms responsible for these changes, including the atomic structure, electronic wavefunctions, and dielectric screening, it combines ab initio calculations with a quantum-embedding approach. By studying various carbon-based defects embedded in monolayer and bulk hBN, it demonstrates that the dominant effect of the change in the environment is the screening of density-density Coulomb interactions between the defect orbitals. The comparative analysis of experimental and theoretical findings paves the way for improved identification of defects in low-dimensional materials and the development of atomic scale sensors for dielectric environments.

Printable two-dimensional superconducting monolayers.

Two-dimensional superconductor (2DSC) monolayers with non-centrosymmetry exhibit unconventional Ising pair superconductivity and an enhanced upper critical field beyond the Pauli paramagnetic limit, driving intense research interest. However, they are often susceptible to structural disorder and environmental oxidation, which destroy electronic coherence and provide technical challenges in the creation of artificial van der Waals heterostructures (vdWHs) for devices. Herein, we report a general and scalable synthesis of highly crystalline 2DSC monolayers via a mild electrochemical exfoliation method using flexible organic ammonium cations solvated with neutral solvent molecules as co-intercalants. Using NbSe2 as a model system, we achieved a high yield (>75%) of large-sized single-crystal monolayers up to 300 µm. The as-fabricated, twisted NbSe2 vdWHs demonstrate high stability, good interfacial properties and a critical current that is modulated by magnetic field when one flux quantum fits to an integer number of moiré cells. Additionally, formulated 2DSC inks can be exploited to fabricate wafer-scale 2D superconducting wire arrays and three-dimensional superconducting composites with desirable morphologies.

Surface State-Dominated Photoconduction and THz Generation in Topological Bi2Te2Se Nanowires.

Topological insulators constitute a fascinating class of quantum materials with nontrivial, gapless states on the surface and insulating bulk states. By revealing the optoelectronic dynamics in the whole range from femto- to microseconds, we demonstrate that the long surface lifetime of Bi2Te2Se nanowires allows us to access the surface states by a pulsed photoconduction scheme and that there is a prevailing bolometric response of the surface states. The interplay of the surface and bulk states dynamics on the different time scales gives rise to a surprising physical property of Bi2Te2Se nanowires: their pulsed photoconductance changes polarity as a function of laser power. Moreover, we show that single Bi2Te2Se nanowires can be used as THz generators for on-chip high-frequency circuits at room temperature. Our results open the avenue for single Bi2Te2Se nanowires as active modules in optoelectronic high-frequency and THz circuits.

Current-Induced Spin Polarization in Topological Insulator-Graphene Heterostructures.

Further development of the field of all-electric spintronics requires the successful integration of spin transport channels with spin injector/generator elements. While with the advent of graphene and related 2D materials high performance spin channel materials are available, the use of nanostructured spin generators remains a major challenge. Especially promising for the latter purpose are 3D topological insulators, whose 2D surface states host massless Dirac Fermions with spin-momentum locking. Here, we demonstrate injection of spin-polarized current from a topological insulator into graphene, enabled by its intimate coupling to an ultrathin Bi2Te2Se nanoplatelet within a van der Waals epitaxial heterostructure. The spin switching signal, whose magnitude scales inversely with temperature, is detectable up to ∼15 K. Our findings establish topological insulators as prospective future components of spintronic devices wherein spin manipulation is achieved by purely electrical means.

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.

Atomic and Electronic Structure of Defects in hBN: Enhancing Single-Defect Functionalities.

Defect centers in insulators play a critical role in creating important functionalities in materials: prototype qubits, single-photon sources, magnetic field probes, and pressure sensors. These functionalities are highly dependent on their midgap electronic structure and orbital/spin wave function contributions. However, in most cases, these fundamental properties remain unknown or speculative due to the defects being deeply embedded beneath the surface of highly resistive host crystals, thus impeding access through surface probes. Here, we directly inspected the atomic and electronic structures of defects in thin carbon-doped hexagonal boron nitride (hBN:C) by using scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS). Such investigation adds direct information about the electronic midgap states to the well-established photoluminescence response (including single-photon emission) of intentionally created carbon defects in the most commonly investigated van der Waals insulator. Our joint atomic-scale experimental and theoretical investigations reveal two main categories of defects: (1) single-site defects manifesting as donor-like states with atomically resolved structures observable via STM and (2) multisite defect complexes exhibiting a ladder of empty and occupied midgap states characterized by distinct spatial geometries. Combining direct probing of midgap states through tunneling spectroscopy with the inspection of the optical response of insulators hosting specific defect structures holds promise for creating and enhancing functionalities realized with individual defects in the quantum limit. These findings underscore not only the versatility of hBN:C as a platform for quantum defect engineering but also its potential to drive advancements in atomic-scale optoelectronics.

Ultrafast exciton fluid flow in an atomically thin MoS2 semiconductor.

Excitons (coupled electron-hole pairs) in semiconductors can form collective states that sometimes exhibit spectacular nonlinear properties. Here, we show experimental evidence of a collective state of short-lived excitons in a direct-bandgap, atomically thin MoS2 semiconductor whose propagation resembles that of a classical liquid as suggested by the nearly uniform photoluminescence through the MoS2 monolayer regardless of crystallographic defects and geometric constraints. The exciton fluid flows over ultralong distances (at least 60 µm) at a speed of ~1.8 × 107 m s-1 (~6% the speed of light). The collective phase emerges above a critical laser power, in the absence of free charges and below a critical temperature (usually Tc ≈ 150 K) approaching room temperature in hexagonal-boron-nitride-encapsulated devices. Our theoretical simulations suggest that momentum is conserved and local equilibrium is achieved among excitons; both these features are compatible with a fluid dynamics description of the exciton transport.

Spin filter effect of hBN/Co detector electrodes in a 3D topological insulator spin valve.

Topological insulators emerge as promising components of spintronic devices, in particular for applications where all-electrical spin control is essential. While the capability of these materials to generate spin-polarized currents is well established, only very little is known about the spin injection/extraction into/out of them. Here, we explore the switching behavior of lateral spin valves comprising the 3D topological insulator Bi2Te2Se as channel, which is separated from ferromagnetic Cobalt detector contacts by an ultrathin hexagonal boron nitride (hBN) tunnel barrier. The corresponding contact resistance displays a notable variation, which is correlated with a change of the switching characteristics of the spin valve. For contact resistances below ~5 kΩ, the hysteresis in the switching curve reverses upon reversing the applied current, as expected for spin-polarized currents carried by the helical surface states. By contrast, for higher contact resistances an opposite polarity of the hysteresis loop is observed, which is independent of the current direction, a behavior signifying negative spin detection efficiency of the multilayer hBN/Co contacts combined with bias-induced spin signal inversion. Our findings suggest the possibility to tune the spin exchange across the interface between a ferromagnetic metal and a topological insulator through the number of intervening hBN layers.

Spin Hall photoconductance in a three-dimensional topological insulator at room temperature.

Three-dimensional topological insulators are a class of Dirac materials, wherein strong spin-orbit coupling leads to two-dimensional surface states. The latter feature spin-momentum locking, i.e., each momentum vector is associated with a spin locked perpendicularly to it in the surface plane. While the principal spin generation capability of topological insulators is well established, comparatively little is known about the interaction of the spins with external stimuli like polarized light. We observe a helical, bias-dependent photoconductance at the lateral edges of topological Bi2Te2Se platelets for perpendicular incidence of light. The same edges exhibit also a finite bias-dependent Kerr angle, indicative of spin accumulation induced by a transversal spin Hall effect in the bulk states of the Bi2Te2Se platelets. A symmetry analysis shows that the helical photoconductance is distinct to common longitudinal photoconductance and photocurrent phenomena, but consistent with optically injected spins being transported in the side facets of the platelets.

Harnessing Topological Band Effects in Bismuth Telluride Selenide for Large Enhancements in Thermoelectric Properties through Isovalent Doping.

Dilute isovalent sulfur doping simultaneously increases electrical conductivity and Seebeck coefficient in Bi2 Te2 Se nanoplates, and bulk pellets made from them. This unusual trend at high electron concentrations is underpinned by multifold increases in electron effective mass attributable to sulfur-induced band topology effects, providing a new way for accessing a high thermoelectric figure-of-merit in topological-insulator-based nanomaterials through doping.

Dimensional crossover in the quantum transport behaviour of the natural topological insulator Aleksite.

Three-dimensional topological insulators comprise topologically protected surface states displaying massless, Dirac-like linear dispersion with spin-momentum locking. Electrical conduction through such surface states has been documented to manifest itself in a two-dimensional character of the angle-dependent magnetotransport behavior. Here, we explore the size-dependent electronic properties of nanostructures made of the lead-containing mineral Aleksite, a naturally occurring topological insulator. Compared to its sister compound Kawazulite, a member of the well-studied Tetradymite crystal class, the crystal structure of Aleksite is distinguished by its lack of any counterpart within the group of synthetic topological insulators. Low temperature Hall measurements on thin Aleksite nanosheets reveal a significant carrier mobility on the order of 1000 cm(2)/(Vs), and a high carrier density of n = 3.9 × 10(25) m(-3). Importantly, for Aleksite nanoribbons with a width below 150 nm, a 1D weak antilocalization effect along with 1D universal conductance fluctuations emerges, which transforms into 2D behavior for larger ribbon widths.