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Transition metal dichalcogenide (TMD) materials have attracted substantial interest due to their remarkable excitonic, optical, electrical, and mechanical properties, which are highly dependent on their crystal structure. Controlling the crystal structure of these materials is essential for fine-tuning their performance, $\textit{e.g.}$, linear and nonlinear optical, as well as charge transport properties. While various phase-switching TMD materials, like molybdenum telluride (MoTe$_2$), are available, their transitions are often irreversible. Here, we investigate the mechanism of a light-induced reversible phase transition in mono- and bilayer flakes of rhenium disulfide (ReS$_2$). Our observations, based on scanning transmission electron microscopy, nonlinear spectroscopy, and density functional theory calculations, reveal a transition from the ground T$''$ (double distorted T) to the metastable H$'$ (distorted H) phase under femtosecond laser irradiation or influence of highly-energetic electrons. We show that the formation of sulfur vacancies facilitates this phenomenon. Our findings pave the way towards actively manipulating the crystal structure of ReS$_2$ and possibly its heterostructures.

We systematically investigate the influence of the fabrication process on dielectric loss in aluminum-on-silicon superconducting coplanar waveguide resonators with internal quality factors ($Q_i$) of about one million at the single-photon level. These devices are essential components in superconducting quantum processors; they also serve as proxies for understanding the energy loss of superconducting qubits. By systematically varying several fabrication steps, we identify the relative importance of reducing loss at the substrate-metal and the substrate-air interfaces. We find that it is essential to clean the silicon substrate in hydrogen fluoride (HF) prior to aluminum deposition. A post-fabrication removal of the oxides on the surface of the silicon substrate and the aluminum film by immersion in HF further improves the $Q_i$. We observe a small, but noticeable, adverse effect on the loss by omitting either standard cleaning (SC1), pre-deposition heating of the substrate to 300$\deg$C, or in-situ post-deposition oxidation of the film's top surface. We find no improvement due to excessive pumping meant to reach a background pressure below $6{\times} 10^{-8}$ mbar. We correlate the measured loss with microscopic properties of the substrate-metal interface through characterization with X-ray photoelectron spectroscopy (XPS), time-of-flight secondary ion mass spectroscopy (ToF-SIMS), transmission electron microscopy (TEM), energy-dispersive X-ray spectroscopy (EDS), and atomic force microscopy (AFM)., Comment: 22 pages, 11 figures

We present a report on hybrid InSb-Pb nanowires that combine high spin-orbit coupling with a high critical field and a large superconducting gap. Material characterization indicates the Pb layer of high crystal quality on the nanowire side facets. Hard induced superconducting gaps and gate-tunable supercurrent are observed in the hybrid nanowires. These results showcase the promising potential of this material combination for a diverse range of applications in hybrid quantum transport devices., Comment: 11 pages, 3 figures

The discovery of van der Waals (vdW) magnetic materials exhibiting non-trivial and tunable magnetic interactions can give rise to exotic magnetic states, which are not readily attainable with conventional materials. Such vdW magnets can provide a unique platform for studying new magnetic phenomena and realizing magnetization dynamics for energy-efficient and non-volatile spintronic memory and computing technologies. Here, we discover the coexistence of ferromagnetic and antiferromagnetic orders in vdW magnet (Co0.5Fe0.5)5-xGeTe2 (CFGT) CFGT above room temperature, inducing an intrinsic exchange bias and canted perpendicular magnetism. Such non-trivial intrinsic magnetic order enables us to realize energy-efficient, magnetic field-free, and deterministic spin-orbit torque (SOT) switching of CFGT in heterostructure with Pt. The devices show a very large spin Hall conductivity, a low critical current density, and yield a large SOT effective field. These experiments, together with density functional theory and Monte Carlo simulations establish coexisting non-trivial magnetic orders in CFGT that enable field-free SOT magnetization dynamics in spintronic devices.

Optical anapoles are intriguing charge-current distributions characterized by a strong suppression of electromagnetic radiation. They originate from the destructive interference of the radiation produced by electric and toroidal multipoles. Although anapoles in dielectric structures have been probed and mapped with a combination of near- and far-field optical techniques, their excitation using fast electron beams has not been explored so far. Here, we theoretically and experimentally analyze the excitation of optical anapoles in tungsten disulfide (WS$_2$) nanodisks using Electron Energy Loss Spectroscopy (EELS) in Scanning Transmission Electron Microscopy (STEM). We observe prominent dips in the electron energy loss spectra and associate them with the excitation of optical anapoles and anapole-exciton hybrids. We are able to map the anapoles excited in the WS$_2$ nanodisks with subnanometer resolution and find that their excitation can be controlled by placing the electron beam at different positions on the nanodisk. Considering current research on the anapole phenomenon, we envision EELS in STEM to become a useful tool for accessing optical anapoles appearing in a variety of dielectric nanoresonators., Comment: 4 figures

We present a fabrication method for reliably and reproducibly forming electrical contacts to 2D materials, based on the tri-layer resist system. We demonstrate the applicability of this method for epitaxial graphene on silicon carbide (epigraphene) and the transition metal dichalcogenides (TMDCs) molybdenum disulfide ($MoS_2$). For epigraphene, the specific contact resistances are of the order of $\rho_c$ ~ $50$ $\Omega\mu m$, and follow the Landauer quantum limit, $\rho_c \propto n^{-1/2}$, with $n$ being the carrier density of graphene. For $MoS_2$ flakes, our edge contacts enable field effect transistors (FET) with ON/OFF ratio of $> 10^6$ at room temperature ( $> 10^9$ at cryogenic temperatures). The fabrication route here demonstrated allows for contact metallization using thermal evaporation and also by sputtering, giving an additional flexibility when designing electrical interfaces, which is key in practical devices and when exploring the electrical properties of emerging materials.

Strain engineering provides an effective way of tailoring the electronic and optoelectronic properties of semiconductor nanomaterials and nanodevices, giving rise to novel functionalities. Here, we present direct experimental evidence of strain-induced modifications of hole mobility in individual GaAs nanowires, using in situ transmission electron microscopy (TEM). The conductivity of the nanowires varied with applied uniaxial tensile stress, showing an initial decrease of ~5-20% up to a stress of 1~ 2 GPa, subsequently increasing up to the elastic limit of the nanowires. This is attributed to a hole mobility variation due to changes in the valence band structure caused by stress and strain. The corresponding lattice strain in the nanowires was quantified by in situ 4D-scanning TEM (STEM) and showed a complex spatial distribution at all stress levels. Meanwhile, a significant red shift of the band gap induced by the stress and strain was unveiled by monochromated electron energy loss spectroscopy.

Second-harmonic generation (SHG) is a direct measure of the strength of second-order nonlinear optical effects, which also include frequency mixing and parametric oscillations. Natural and artificial materials with broken center-of-inversion symmetry in their unit cell display high SHG efficiency, however the silicon-foundry compatible group-IV semiconductors (Si, Ge) are centrosymmetric, thereby preventing full integration of second-order nonlinearity in silicon photonics platforms. Here we demonstrate strong SHG in Ge-rich quantum wells grown on Si wafers. The symmetry breaking is artificially realized with a pair of asymmetric coupled quantum wells (ACQW), in which three of the quantum-confined states are equidistant in energy, resulting in a double resonance for SHG. Laser spectroscopy experiments demonstrate a giant second-order nonlinearity at mid-infrared pump wavelengths between 9 and 12 microns. Leveraging on the strong intersubband dipoles, the nonlinear susceptibility almost reaches 10^5 pm/V, Comment: 30 pages, 6 figures, double line spacing

Semiconductor-superconductor hybrids are widely used for realising complex quantum phenomena such as topological superconductivity and spins coupled to Cooper pairs. Accessing exotic regimes at high magnetic fields and increasing operating temperatures beyond the state-of-the-art requires new, epitaxially matched semiconductor-superconductor materials. The challenge is to generate favourable conditions for heterostructure formation between materials with the desired inherent properties. Here, we harness increased knowledge of metal-on-semiconductor growth to develop InAs nanowires with epitaxially matched, single crystal, atomically flat Pb films along the entire nanowire. These highly ordered heterostructures have a critical temperature of 7 K and a superconducting gap of 1.25 meV, which remains hard at 8.5 T, thereby more than doubling the available parameter space. Additionally, InAs/Pb island devics exhibit magnetic field-driven transitions from Cooper pair to single electron charging; a pre-requisite for use in topological quantum computation. Introducing semiconductor-Pb hybrids potentially enables access to entirely new regimes for an array of quantum systems.

The ability to extract materials just a few atoms thick has led to discovery of graphene, monolayer transition metal dichalcogenides (TMDs), and other important two-dimensional materials. The next step in promoting understanding and utility of the flatland physics beyond the state-of-the-art is to study one-dimensional edges of such two-dimensional materials as well as to control the edge-plane ratio. Edges typically exhibit properties that are unique and distinctly different from those of planes and bulk. Thus, controlling them allows to design principally new materials with synthetic edge-plane-bulk characteristics, that is, TMD metamaterials. However, the enabling technology to study such metamaterials experimentally in a precise and systematic way has not yet been developed. Here we report a facile and controllable anisotropic wet etching method that allows scalable fabrication of TMD metamaterials with atomic precision. We show that TMDs can be etched along certain crystallographic axes, such that the obtained edges are atomically sharp and exclusively zigzag-terminated. This results in hexagonal nanostructures of predefined order and complexity, including few nanometer thin nanoribbons and nanojunctions. The method thus enables future studies of a broad range of TMD metamaterials with tailored functionality through atomically precise control of the structure.

Kinetic Monte Carlo (KMC) simulations are a powerful tool to study the dynamics of charge carriers in organic photovoltaics. However, the key characteristic of any photovoltaic device, its current-voltage ($J$-$V$) curve under solar illumination, has proven challenging to simulate using KMC. The main challenges arise from the presence of injecting contacts and the importance of charge recombination when the internal electric field is low, i.e., close to open-circuit conditions. In this work, an experimentally calibrated KMC model is presented that can fully predict the $J$-$V$ curve of a disordered organic solar cell. It is shown that it is crucial to make experimentally justified assumptions on the injection barriers, the blend morphology, and the kinetics of the charge transfer state involved in geminate and nongeminate recombination. All of these properties are independently calibrated using charge extraction, electron microscopy, and transient absorption measurements, respectively. Clear evidence is provided that the conclusions drawn from microscopic and transient KMC modeling are indeed relevant for real operating organic solar cell devices., Comment: final version; license updated

Polaritons are compositional light-matter quasiparticles that have recently enabled remarkable breakthroughs in quantum and nonlinear optics, as well as in material science. Despite the enormous progress, however, a direct nanometer-scale visualization of polaritons has remained an open challenge. Here, we demonstrate that plasmon-exciton polaritons, or plexcitons, generated by a hybrid system composed of an individual silver nanoparticle and a few-layer transition metal dichalcogenide can be spectroscopically mapped with nanometer spatial resolution using electron energy loss spectroscopy in a scanning transmission electron microscope. Our experiments reveal important insights about the coupling process, which have not been reported so far. These include nanoscale variation of Rabi splitting and plasmon-exciton detuning, as well as absorption-dominated extinction signals, which in turn provide the ultimate evidence for the plasmon-exciton hybridization in the strong coupling regime. These findings pioneer new possibilities for in-depth studies of polariton-related phenomena with nanometer spatial resolution.

While it is well established that elevated temperatures can induce surface roughening of metal surfaces, the effect of a high electric field on the atomic structure at ambient temperature has not been investigated in detail. Here we show with atomic resolution using in situ transmission electron microscopy how intense electric fields induce reversible switching between perfect crystalline and disordered phases of gold surfaces at room temperature. Ab initio molecular dynamics simulations reveal that the mechanism behind the structural change can be attributed to a vanishing energy cost in forming surface defects in high electric fields. Our results demonstrate how surface processes can be directly controlled at the atomic scale by an externally applied electric field, which promotes an effective decoupling of the topmost surface layers from the underlying bulk. This opens up opportunities for development of active nanodevices in e.g. nanophotonics and field-effect transistor technology as well as fundamental research in materials characterization and of yet unexplored dynamically-controlled low-dimensional phases of matter., Comment: The manuscript is 10 pages long and the supplemental material is 15 pages. There are six supplemental movies that can be provided upon request to LDK

Topological superconductivity is central to a variety of novel phenomena involving the interplay between topologically ordered phases and broken-symmetry states. The key ingredient is an unconventional order parameter, with an orbital component containing a chiral $p_x$ + i$p_y$ wave term. Here we present phase-sensitive measurements, based on the quantum interference in nanoscale Josephson junctions, realized by using Bi$_2$Te$_3$ topological insulator. We demonstrate that the induced superconductivity is unconventional and consistent with a sign-changing order parameter, such as a chiral $p_x$ + i$p_y$ component. The magnetic field pattern of the junctions shows a dip at zero externally applied magnetic field, which is an incontrovertible signature of the simultaneous existence of 0 and $\pi$ coupling within the junction, inherent to a non trivial order parameter phase. The nano-textured morphology of the Bi$_2$Te$_3$ flakes, and the dramatic role played by thermal strain are the surprising key factors for the display of an unconventional induced order parameter., Comment: 47 pages, 7 figures in the main text and 12 figures in the supplementary material

In this study we investigate the functional behavior of the intensity in high-angle annular dark field (HAADF) scanning transmission electron micrograph (STEM) images. The model material is a silica particle (20 nm) gel at 5 wt%. By assuming that the intensity response is monotonically increasing with increasing mass thickness of silica, an estimate of the functional form is calculated using a maximum likelihood approach. We conclude that a linear functional form of the intensity provides a fair estimate but that a power function is significantly better for estimating the amount of silica in the z-direction. The work adds to the development of quantifying material properties from electron micrographs, especially in the field of tomography methods and three-dimensional quantitative structural characterization from a STEM micrograph. It also provides means for direct three-dimensional quantitative structural characterization from a STEM micrograph.

We have developed a new method to fabricate biepitaxial YBa2Cu3O(7-x) (YBCO) Josephson junctions at the nanoscale, allowing junctions widths down to 100 nm and simultaneously avoiding the typical damage in grain boundary interfaces due to conventional patterning procedures. By using the competition between the superconducting YBCO and the insulating Y2BaCuO5 phases during film growth, we formed nanometer sized grain boundary junctions in the insulating Y2BaCuO5 matrix as confirmed by high resolution transmission electron microscopy. Electrical transport measurements give clear indications that we are close to probing the intrinsic properties of the grain boundaries., Comment: 16 pages, 6 figures

We demonstrate the quantitative measurement of the magnetization of individual magnetic nanoparticles (MNP) using a magnetic force microscope (MFM). The quantitative measurement is realized by calibration of the MFM signal using an MNP reference sample with traceably determined magnetization. A resolution of the magnetic moment of the order of 10^(-18) Am^2 under ambient conditions is demonstrated which is presently limited by the tip's magnetic moment and the noise level of the instrument. The calibration scheme can be applied to practically any MFM and tip thus allowing a wide range of future applications e.g. in nanomagnetism and biotechnology., Comment: 12 pages, 3 figures