High Magnetic Field Stability in a Planar Graphene-NbSe2 SQUID.

Thin NbSe2 retains superconductivity at a high in-plane magnetic field up to 30 T. In this work we construct a novel atomically thin, all van der Waals SQUID, in which current flows between NbSe2 contacts through two parallel graphene weak links. The 2D planar SQUID remains uniquely stable at high in-plane field, which enables tracing critical current interference patterns as a function of the field up to 4.5 T. From these we extract the evolution of the current distribution up to high fields, demonstrating sub-nanometer sensitivity to deviation of current flow from a perfect atomic plane and observing a field-driven transition in which supercurrent redistributes to a narrow channel. We further suggest a new application of the asymmetric SQUID geometry to directly probe the current density in the absence of phase information.

Nano-Patterned Magnetic Edges in CrGeTe3 for Quasi 1-D Spintronic Devices.

The synthesis of two-dimensional van der Waals magnets has paved the way for both technological applications and fundamental research on magnetism confined to ultra-small length scales. Edge magnetic moments in ferromagnets are expected to be less magnetized than in the sample interior because of the reduced amount of neighboring ferromagnetic spins at the sample edge. We recently demonstrated that CrGeTe3 (CGT) flakes thinner than 10 nm are hard ferromagnets; i.e., they exhibit an open hysteresis loop. In contrast, thicker flakes exhibit zero net remnant field in the interior, with hard ferromagnetism present only at the cleaved edges. This experimental observation suggests that a nontrivial interaction exists between the sample edge and the interior. Here, we demonstrate that artificial edges fabricated by focus ion beam etching also display hard ferromagnetism. This enables us to write magnetic nanowires in CGT directly and use this method to characterize the magnetic interaction between the interior and edge. The results indicate that the interior saturation and depolarization fields depend on the lateral dimensions of the sample. Most notably, the interior region between the edges of a sample narrower than 300 nm becomes a hard ferromagnet, suggesting an enhancement of the magnetic exchange induced by the proximity of the edges. Last, we find that the CGT regions amorphized by the gallium beam are nonmagnetic, which introduces a novel method to tune the local magnetic properties of CGT films, potentially enabling integration into spintronic devices.

Thickness Mapping and Layer Number Identification of Exfoliated van der Waals Materials by Fourier Imaging Micro-Ellipsometry.

As performance of van der Waals heterostructure devices is governed by the nanoscale thicknesses and homogeneity of their constituent mono- to few-layer flakes, accurate mapping of these properties with high lateral resolution becomes imperative. Spectroscopic ellipsometry is a promising optical technique for such atomically thin-film characterization due to its simplicity, noninvasive nature and high accuracy. However, the effective use of standard ellipsometry methods on exfoliated micron-scale flakes is inhibited by their tens-of-microns lateral resolution or slow data acquisition. In this work, we demonstrate a Fourier imaging spectroscopic micro-ellipsometry method with sub-5 µm lateral resolution and three orders-of-magnitude faster data acquisition than similar-resolution ellipsometers. Simultaneous recording of spectroscopic ellipsometry information at multiple angles results in a highly sensitive system, which is used for performing angstrom-level accurate and consistent thickness mapping on exfoliated mono-, bi- and trilayers of graphene, hexagonal boron nitride (hBN) and transition metal dichalcogenide (MoS2, WS2, MoSe2, WSe2) flakes. The system can successfully identify highly transparent monolayer hBN, a challenging proposition for other characterization tools. The optical microscope integrated ellipsometer can also map minute thickness variations over a micron-scale flake, revealing its lateral inhomogeneity. The prospect of adding standard optical elements to augment generic optical imaging and spectroscopy setups with accurate in situ ellipsometric mapping capability presents potential opportunities for investigation of exfoliated 2D materials.

Chip-Integrated Vortex Manipulation.

The positions of Abrikosov vortices have long been considered as means to encode classical information. Although it is possible to move individual vortices using local probes, the challenge of scalable on-chip vortex-control remains outstanding, especially when considering the demands of controlling multiple vortices. Realization of vortex logic requires means to shuttle vortices reliably between engineered pinning potentials, while concomitantly keeping all other vortices fixed. We demonstrate such capabilities using Nb loops patterned below a NbSe2 layer. SQUID-on-Tip (SOT) microscopy reveals that the loops localize vortices in designated sites to a precision better than 100 nm; they realize "push" and "pull" operations of vortices as far as 3 µm. Successive application of such operations shuttles a vortex between adjacent loops. Our results may be used as means to integrate vortices in future quantum circuitry. Strikingly, we demonstrate a winding operation, paving the way for future topological quantum computing and simulations.

Creation of Boron Vacancies in Hexagonal Boron Nitride Exfoliated from Bulk Crystals for Quantum Sensing.

Boron vacancies (VB-) in hexagonal boron -nitride (hBN) have sparked great interest in recent years due to their optical and spin properties. Since hBN can be readily integrated into devices where it interfaces a huge variety of other 2D materials, boron vacancies may serve as a precise sensor which can be deployed at very close proximity to many important materials systems. Boron vacancy defects may be produced by a number of existing methods, the use of which may depend on the final application. Any method should reproducibly generate defects with controlled density and desired pattern. To date, however, detailed studies of such methods are missing. In this paper, we study various techniques for the preparation of hBN flakes from bulk crystals and relevant postprocessing treatments, namely, focused ion beam (FIB) implantation, for creation of VB-s as a function of flake thickness and defect concentrations. We find that flake thickness plays an important role when optimizing implantation parameters, while careful sample cleaning proved important to achieve consistent results.

Interior and Edge Magnetization in Thin Exfoliated CrGeTe3 Films.

CrGeTe3 (CGT) is a semiconducting vdW ferromagnet shown to possess magnetism down to a two-layer thick sample. Although CGT is one of the leading candidates for spintronics devices, a comprehensive analysis of CGT thickness dependent magnetization is currently lacking. In this work, we employ scanning SQUID-on-tip (SOT) microscopy to resolve the magnetic properties of exfoliated CGT flakes at 4.2 K. Combining transport measurements of CGT/NbSe2 samples with SOT images, we present the magnetic texture and hysteretic magnetism of CGT, thereby matching the global behavior of CGT to the domain structure extracted from local SOT magnetic imaging. Using this method, we provide a thickness dependent magnetization state diagram of bare CGT films. No zero-field magnetic memory was found for films thicker than 10 nm, and hard ferromagnetism was found below that critical thickness. Using scanning SOT microscopy, we identify a unique edge magnetism, contrasting the results attained in the CGT interior.

Positron charge sensing using a double-gated graphene field effect transistor.

We utilize a high-mobility double-gated graphene field-effect transistor to measure the accumulated charge created by positron annihilation in its back-gate. The device consists of an exfoliated graphene flake stacked between two hexagonal boron nitride flakes placed on a 1 cm2 substrate of 500 µm thick conducting p-doped Si capped by 285 nm-thick SiO2. The device is placed in close proximity to a 780 kBq 22Na positron source emitting a constant flux of positrons. During the measurement, positrons annihilate within the back-gate, kept floating using a low-capacitance relay. The accumulated positive charge capacitively couples to the graphene device and builds a positive voltage, detectable through a shift in the top-gate dependent graphene resistance characteristic. The shift in the position of the top-gate Dirac peak is then used for extracting the exact voltage buildup and quantitative evaluation of the accumulated charge. Reaching a positron current sensitivity of ∼1.2 fA/Hz, detected over 20 min, our results demonstrate the utility of two-dimensional layered materials as probes for charging dynamics of positrons in solids.

Spectroscopy of NbSe2 Using Energy-Tunable Defect-Embedded Quantum Dots.

Quantum dots have sharply defined energy levels, which can be used for high resolution energy spectroscopy when integrated in tunneling circuitry. Here we report dot-assisted spectroscopy measurements of the superconductor NbSe2, using a van der Waals device consisting of a vertical stack of graphene-MoS2-NbSe2. The MoS2 tunnel barriers host naturally occurring defects which function as quantum dots, allowing transport via resonant tunneling. The dot energies are tuned by an electric field exerted by a back-gate, which penetrates the graphene source electrode. Scanning the dot potential across the superconductor Fermi energy, we reproduce the NbSe2 density of states which exhibits a well-resolved two-gap spectrum. Surprisingly, we find that the dot-assisted current is dominated by the lower energy feature of the two NbSe2 gaps, possibly due to a selection rule which favors coupling between the dots and the orbitals which exhibit this gap.

Quantum-dot assisted spectroscopy of degeneracy-lifted Landau levels in graphene.

Energy spectroscopy of strongly interacting phases requires probes which minimize screening while retaining spectral resolution and local sensitivity. Here, we demonstrate that such probes can be realized using atomic sized quantum dots bound to defects in hexagonal Boron Nitride tunnel barriers, placed at nanometric distance from graphene. With dot energies capacitively tuned by a planar graphite electrode, dot-assisted tunneling becomes highly sensitive to the graphene excitation spectrum. The spectra track the onset of degeneracy lifting with magnetic field at the ground state, and at unoccupied excited states, revealing symmetry-broken gaps which develop steeply with magnetic field - corresponding to Landé g factors as high as 160. Measured up to B = 33 T, spectra exhibit a primary energy split between spin-polarized excited states, and a secondary spin-dependent valley-split. Our results show that defect dots probe the spectra while minimizing local screening, and are thus exceptionally sensitive to interacting states.

Quantum Phase Transitions of Trilayer Excitons in Atomically Thin Heterostructures.

We determine the phase diagram of excitons in a symmetric transition-metal dichalcogenide 3-layer heterostructure. First principles calculations reveal interlayer exciton states of a symmetric quadrupole, from which higher energy asymmetric dipole states are composed. We find quantum phase transitions between a repulsive quadrupolar and an attractive staggered dipolar lattice phases, driven by a competition between interactions and single exciton energies. The different internal quantum state of excitons in each phase is a striking example of a system where single-particle and interacting many-body states are coupled.

Observation of 2D semiconductor P-type dark-exciton lifetime using two-photon ultrafast spectroscopy.

We report direct measurements of intrinsic lifetimes of P-type dark-excitons in MoS2 monolayers. Using sub-gap excitation, we demonstrate two-photon excited direct population of P-type dark excitons, observe their scattering to bright states and decay with femtosecond resolution. In contrast to one-photon excitation schemes, non-monotonic density variation in bright exciton population observed under two-photon excitation shows the indirect nature of its population and competing decay pathways. Detailed modeling of different recombination pathways of bright and dark excitons allows experimental measurement of 2P dark → 1S bright exciton scattering rates. These insights into the dark states in a MoS2 monolayer pave the way for novel devices such as quantum memories and computing.

Zeeman Tunability of Andreev Bound States in van der Waals Tunnel Barriers.

Quantum dots proximity coupled to superconductors are attractive research platforms due to the intricate interplay between the single-electron nature of the dot and the many body nature of the superconducting state. These have been studied mostly using nanowires and carbon nanotubes, which allow a combination of tunability and proximity. Here we report a new type of quantum dot which allows proximity to a broad range of superconducting systems. The dots are realized as embedded defects within semiconducting tunnel barriers in van der Waals layers. By placing such layers on top of thin NbSe_{2}, we can probe the Andreev bound state spectra of such dots up to high in-plane magnetic fields without observing the effects of a diminishing superconducting gap. As tunnel junctions defined on NbSe_{2} have a hard gap, we can map the subgap spectra without a background related to the rest of the junction. We find that the proximitized defect states invariably have a singlet ground state, manifest in the Zeeman splitting of the subgap excitation. We also find, in some cases, bound states that converge to zero energy and remain there. We discuss the role of the spin-orbit term, present both in the barrier and the superconductor, in the realization of such topologically trivial zero-energy states.

Magnetic-related States and Order Parameter Induced in a Conventional Superconductor by Nonmagnetic Chiral Molecules.

Hybrid ferromagnetic/superconducting systems are well-known for hosting intriguing phenomena such as emergent triplet superconductivity at their interfaces and the appearance of in-gap, spin-polarized Yu-Shiba-Rusinov (YSR) states bound to magnetic impurities on a superconducting surface. In this work we demonstrate that similar phenomena can be induced on a surface of a conventional superconductor by chemisorbing nonmagnetic chiral molecules. Conductance spectra measured on NbSe2 flakes over which chiral α-helix polyalanine molecules were adsorbed exhibit, in some cases, in-gap states nearly symmetrically positioned around zero bias that shift with magnetic field, akin to YSR states, as corroborated by theoretical simulations. Other samples show evidence for a collective phenomenon of hybridized YSR-like states giving rise to unconventional, possibly triplet superconductivity, manifested in the conductance spectra by the appearance of a zero bias conductance that diminishes, but does not split, with magnetic field. The transition between these two scenarios appears to be governed by the density of adsorbed molecules.

Tunneling into the Vortex State of NbSe2 with van der Waals Junctions.

We have performed device-based tunneling spectroscopy of NbSe2 in the vortex state with a magnetic field applied both parallel and perpendicular to the a- b plane. Our devices consist of layered semiconductors placed on top of exfoliated NbSe2 using the van der Waals transfer technique. At zero field, the spectrum exhibits a hard gap, and the quasiparticle peak is split into low- and high-energy features. The two features, associated with the effective two-band nature of superconductivity in NbSe2, exhibit markedly distinct responses to the application of magnetic field, suggesting an order-of-magnitude difference in the spatial extent of the vortex cores of the two bands. At energies below the superconducting gap, the hard gap gives way to vortex-bound Caroli-de Gennes-Matricon states, allowing the detection of individual vortices as they enter and exit the junction. Analysis of the subgap spectra upon application of parallel magnetic field allows us to track the process of vortex surface formation and spatial rearrangement in the bulk.

Bidirectional Soliton Rain Dynamics Induced by Casimir-Like Interactions in a Graphene Mode-Locked Fiber Laser.

We study experimentally and theoretically the interactions among ultrashort optical pulses in the soliton rain multiple-pulse dynamics of a fiber laser. The laser is mode locked by a graphene saturable absorber fabricated using the mechanical transfer technique. Dissipative optical solitons aggregate into pulse bunches that exhibit complex behavior, which includes acceleration and bidirectional motion in the moving reference frame. The drift speed and direction depend on the bunch size and relative location in the cavity, punctuated by abrupt changes under bunch collisions. We model the main effects using the recently proposed noise-mediated pulse interaction mechanism, and obtain a good agreement with experiments. This highlights the major role of long-range Casimir-like interactions over dynamical pattern formations within ultrafast lasers.

Electrostatic coupling between two surfaces of a topological insulator nanodevice.

We report on electronic transport measurements of dual-gated nanodevices of the low-carrier density topological insulator (TI) Bi_{1.5}Sb_{0.5}Te_{1.7}Se_{1.3}. In all devices, the upper and lower surface states are independently tunable to the Dirac point by the top and bottom gate electrodes. In thin devices, electric fields are found to penetrate through the bulk, indicating finite capacitive coupling between the surface states. A charging model allows us to use the penetrating electric field as a measurement of the intersurface capacitance C_{TI} and the surface state energy-density relationship µ(n), which is found to be consistent with independent angle-resolved photoemission spectroscopy measurements. At high magnetic fields, increased field penetration through the surface states is observed, strongly suggestive of the opening of a surface state band gap due to broken time-reversal symmetry.

Exchange-coupling-induced symmetry breaking in topological insulators.

An exchange gap in the Dirac surface states of a topological insulator (TI) is necessary for observing the predicted unique features such as the topological magnetoelectric effect as well as to confine Majorana fermions. We experimentally demonstrate proximity-induced ferromagnetism in a TI, combining a ferromagnetic insulator EuS layer with Bi(2)Se(3), without introducing defects. By magnetic and magnetotransport studies, including anomalous Hall effect and magnetoresistance measurements, we show the emergence of a ferromagnetic phase in TI, a step forward in unveiling their exotic properties.

Surface state transport and ambipolar electric field effect in Bi2Se3 nanodevices.

Electronic transport experiments involving the topologically protected states found at the surface of Bi2Se3 and other topological insulators require fine control over carrier density, which is challenging with existing bulk-doped material. Here we report on electronic transport measurements on thin (<100 nm) Bi2Se3 devices and show that the density of the surface states can be modulated via the electric field effect by using a top-gate with a high-k dielectric insulator. The conductance dependence on geometry, gate voltage, and temperature all indicate that transport is governed by parallel surface and bulk contributions. Moreover, the conductance dependence on top-gate voltage is ambipolar, consistent with tuning between electrons and hole carriers at the surface.

Electrical current switching in single CdSe nanorods.

Electrical current measurements through individually wired colloidal CdSe nanorods exhibit pronounced multistability. This current switching is analogous to the widely observed fluorescence intermittency in similar systems and may be associated with surface charge dynamics. Such association is quantitatively established for the case when the current is bistable, where the probability of the sojourn time t at the high or low current state follows an exponential dependence. Remarkably, this behavior can be modeled by charging dynamics of a single surface trap, whose position could be estimated from the intermittent current-voltage characteristics. The methodology presented here provides a unique route for charge dynamic sensing at the nanoscale, where the nanorod senses its own surface charge.

Anomalous temperature dependent transport through single colloidal nanorods strongly coupled to metallic leads.

We report wiring of individual colloidal nanorods (NRs), 30-60 nm long by 3.5-5 nm diameter. Strong electrical coupling is achieved by electron beam induced deposition (EBID) of metallic lines targeting NR tips with nanometric precision. At T = 4 K many devices exhibit smooth I(V) curves with no sharp onset features, which remarkably fit a Fowler-Nordheim tunneling model. All devices exhibit an anomalous exponential temperature dependence of the form I approximately exp(T/T(0)). This irregular behavior cannot be explained by any hopping or activation model and is interpreted by accounting for the lowering of the NR conduction band due to lattice dilation and phonon coupling.