Selective Control of Phases and Electronic Structures of Monolayer TaTe2.

Transition metal dichalcogenide (TMDC) films exhibit rich phases and superstructures, which can be controlled by the growth conditions as well as post-growth annealing treatment. Here, the selective growth of monolayer TaTe2 films with different phases as well as superstructures using molecular beam epitaxy (MBE) is reported. Monolayer 1H-TaTe2 and 1T-TaTe2 films can be selectively controlled by varying the growth temperature, and their different electronic structures are revealed through the combination of angle-resolved photoemission spectroscopy measurements (ARPES) and first-principles calculations. Moreover, post-growth annealing of the 1H-TaTe2 film further leads to a transition from a 19 × 19 $\sqrt {19}{\times }\sqrt {19}$ superstructure to a new 2 × 2 superstructure, where two gaps are observed in the electronic structure and persist up to room temperature. First-principles calculations reveal the role of the phonon instability in the formation of superstructures and the effect of local atomic distortions on the modified electronic structures. This work demonstrates the manipulation of the rich phases and superstructures of monolayer TaTe2 films by controlling the growth kinetics and post-growth annealing.

Nanoscale multistate resistive switching in WO3 through scanning probe induced proton evolution.

Multistate resistive switching device emerges as a promising electronic unit for energy-efficient neuromorphic computing. Electric-field induced topotactic phase transition with ionic evolution represents an important pathway for this purpose, which, however, faces significant challenges in device scaling. This work demonstrates a convenient scanning-probe-induced proton evolution within WO3, driving a reversible insulator-to-metal transition (IMT) at nanoscale. Specifically, the Pt-coated scanning probe serves as an efficient hydrogen catalysis probe, leading to a hydrogen spillover across the nano junction between the probe and sample surface. A positively biased voltage drives protons into the sample, while a negative voltage extracts protons out, giving rise to a reversible manipulation on hydrogenation-induced electron doping, accompanied by a dramatic resistive switching. The precise control of the scanning probe offers the opportunity to manipulate the local conductivity at nanoscale, which is further visualized through a printed portrait encoded by local conductivity. Notably, multistate resistive switching is successfully demonstrated via successive set and reset processes. Our work highlights the probe-induced hydrogen evolution as a new direction to engineer memristor at nanoscale.

Oscillation of Electronic-Band-Gap Size Induced by Crystalline Symmetry Change in Ultrathin PbTe Films.

For the semiconductors of atomic length scales, even one atom layer difference could modify crystal symmetry and lead to a significant change in electronic structure, which is essential for modern electronics. However, the experimental exploration of such effect has not been achieved due to challenges in sample fabrication and characterization with atomic-scale precision. Here, we report the discovery of crystal symmetry alternation induced band-gap oscillation in atomically thin PbTe films by scanning tunneling microscopy. As the thickness of PbTe films is reduced from an 18- to 2-atomic layer, the band-gap size not only expands from 0.19 eV to 1.06 eV by 5.6 fold, but also exhibits an even-odd-layer oscillation, which is attributed to the alternating crystal symmetries between P4/mmm and P4/nmm. Our work sheds new light on electronic structure engineering of semiconductors at atomic scale for next-generation nanoelectronics.

Construction of molecular beam epitaxy and multi-probe scanning tunneling potentiometry combined system.

Molecular beam epitaxy (MBE) is a powerful technique to grow high quality thin films with atomic precision, and multiprobe scanning tunneling potentiometry (STP) is an ideal tool to probe electronic transportation in nanometer scale. We combine the two advanced techniques together and successfully construct a unique system of MBE, STP, and four-probe in situ transport measurement. Excellent functions of this system have been demonstrated by experiments on several materials under ultrahigh vacuum conditions. The system provides an ideal platform for in situ study of electronic transport properties of various thin films, such as two-dimensional superconductors and topological insulators.

Standing Waves Induced by Valley-Mismatched Domains in Ferroelectric SnTe Monolayers.

Two-dimensional (2D) quasiparticle standing waves originate from the interference of coherent quantum states and are usually created by the scattering off edges, atomic steps, or adatoms that induce large potential barriers. We report standing waves close to the valence band maximum (E_{V}), confined by electrically neutral domain walls of newly discovered ferroelectric SnTe monolayers, as revealed by spatially resolved scanning tunneling spectroscopy. Ab initio calculations show that this novel confinement arises from the polarization lifted hole valley degeneracy and a ∼90° rotation of the Brillouin zones that render holes' momentum mismatched across neighboring domains. These results show a potential for polarization-tuned valleytronics in 2D ferroelectrics.

Enhanced Spontaneous Polarization in Ultrathin SnTe Films with Layered Antipolar Structure.

2D SnTe films with a thickness of as little as 2 atomic layers (ALs) have recently been shown to be ferroelectric with in-plane polarization. Remarkably, they exhibit transition temperatures (Tc ) much higher than that of bulk SnTe. Here, combining molecular beam epitaxy, variable temperature scanning tunneling microscopy, and ab initio calculations, the underlying mechanism of the Tc enhancement is unveiled, which relies on the formation of γ-SnTe, a van der Waals orthorhombic phase with antipolar inter-layer coupling in few-AL thick SnTe films. In this phase, 4n - 2 AL (n = 1, 2, 3…) thick films are found to possess finite in-plane polarization (space group Pmn21 ), while 4n AL thick films have zero total polarization (space group Pnma). Above 8 AL, the γ-SnTe phase becomes metastable, and can convert irreversibly to the bulk rock salt phase as the temperature is increased. This finding unambiguously bridges experiments on ultrathin SnTe films with predictions of robust ferroelectricity in GeS-type monochalcogenide monolayers. The observed high transition temperature, together with the strong spin-orbit coupling and van der Waals structure, underlines the potential of atomically thin γ-SnTe films for the development of novel spontaneous polarization-based devices.

Discovery of robust in-plane ferroelectricity in atomic-thick SnTe.

Stable ferroelectricity with high transition temperature in nanostructures is needed for miniaturizing ferroelectric devices. Here, we report the discovery of the stable in-plane spontaneous polarization in atomic-thick tin telluride (SnTe), down to a 1-unit cell (UC) limit. The ferroelectric transition temperature T(c) of 1-UC SnTe film is greatly enhanced from the bulk value of 98 kelvin and reaches as high as 270 kelvin. Moreover, 2- to 4-UC SnTe films show robust ferroelectricity at room temperature. The interplay between semiconducting properties and ferroelectricity in this two-dimensional material may enable a wide range of applications in nonvolatile high-density memories, nanosensors, and electronics.

Thickness Dependence of the Quantum Anomalous Hall Effect in Magnetic Topological Insulator Films.

The evolution of the quantum anomalous Hall effect with the thickness of Cr-doped (Bi,Sb)2 Te3 magnetic topological insulator films is studied, revealing how the effect is caused by the interplay of the surface states, band-bending, and ferromagnetic exchange energy. Homogeneity in ferromagnetism is found to be the key to high-temperature quantum anomalous Hall material.

Observation of Double-Dome Superconductivity in Potassium-Doped FeSe Thin Films.

We report on the emergence of two disconnected superconducting domes in alkali-metal potassium- (K-)doped FeSe ultrathin films grown on graphitized SiC(0001). The superconductivity exhibits hypersensitivity to K dosage in the lower-T_{c} dome, whereas in the heavily electron-doped higher-T_{c} dome it becomes spatially homogeneous and robust against disorder, supportive of a conventional Cooper-pairing mechanism. Furthermore, the heavily K-doped multilayer FeSe films all reveal a large superconducting gap of ∼14 meV, irrespective of film thickness, verifying the higher-T_{c} superconductivity only in the topmost FeSe layer. The unusual finding of a double-dome superconducting phase is a step towards the mechanistic understanding of superconductivity in FeSe-derived superconductors.

Mapping the Electronic Structure of Each Ingredient Oxide Layer of High-T\{c} Cuprate Superconductor Bi{2}Sr{2}CaCu{2}O{8+δ}.

Understanding the mechanism of high transition temperature (T{c}) superconductivity in cuprates has been hindered by the apparent complexity of their multilayered crystal structure. Using a cryogenic scanning tunneling microscopy (STM), we report on layer-by-layer probing of the electronic structures of all ingredient planes (BiO, SrO, CuO{2}) of Bi{2}Sr{2}CaCu_2}O{8+δ} superconductor prepared by argon-ion bombardment and annealing technique. We show that the well-known pseudogap (PG) feature observed by STM is inherently a property of the BiO planes and thus irrelevant directly to Cooper pairing. The SrO planes exhibit an unexpected van Hove singularity near the Fermi level, while the CuO{2} planes are exclusively characterized by a smaller gap inside the PG. The small gap becomes invisible near T{c}, which we identify as the superconducting gap. The above results constitute severe constraints on any microscopic model for high T{c} superconductivity in cuprates.

Probing Dirac fermion dynamics in topological insulator Bi2Se3 films with a scanning tunneling microscope.

Scanning tunneling microscopy and spectroscopy have been used to investigate the femtosecond dynamics of Dirac fermions in the topological insulator Bi2Se3 ultrathin films. At the two-dimensional limit, bulk electrons become quantized and the quantization can be controlled by the film thickness at a single quintuple layer level. By studying the spatial decay of standing waves (quasiparticle interference patterns) off steps, we measure directly the energy and film thickness dependence of the phase relaxation length lϕ and inelastic scattering lifetime τ of topological surface-state electrons. We find that τ exhibits a remarkable (E - EF)(-2) energy dependence and increases with film thickness. We show that the features revealed are typical for electron-electron scattering between surface and bulk states.

Scanning tunneling microscopy studies of topological insulators.

Scanning tunneling microscopy (STM), with surface sensitivity, is an ideal tool to probe the intriguing properties of the surface state of topological insulators (TIs) and topological crystalline insulators (TCIs). We summarize the recent progress on those topological phases revealed by STM studies. STM observations have directly confirmed the existence of the topological surface states and clearly revealed their novel properties. We also discuss STM work on magnetic doped TIs, topological superconductors and crystalline symmetry-protected surface states in TCIs. The studies have greatly promoted our understanding of the exotic properties of the new topological phases, as well as put forward new challenges. STM will continue to play an important role in this rapidly growing field from the point view of both fundamental physics and applications.

Molecular beam epitaxy growth and post-growth annealing of FeSe films on SrTiO3: a scanning tunneling microscopy study.

Low temperature scanning tunneling microscopy and spectroscopy are used to investigate the atomic and electronic structure evolution of FeSe films grown on SrTiO3 as a function of post-growth annealing. Single unit cell FeSe films are found to bond strongly with the underlying substrate, and become superconductive with diminishing chemical bond disorders at the interface via post-annealing. For thicker FeSe films, post-annealing removes excess Se in the films and leads to a transition from semiconductor into metallic behaviors. In double and multilayer films, strain-induced complex textures are observed and suggested to be the main cause for the absent superconductivity.

Atomic-scale transport in epitaxial graphene.

The high carrier mobility of graphene is key to its applications, and understanding the factors that limit mobility is essential for future devices. Yet, despite significant progress, mobilities in excess of the 2×10(5) cm(2) V(-1) s(-1) demonstrated in free-standing graphene films have not been duplicated in conventional graphene devices fabricated on substrates. Understanding the origins of this degradation is perhaps the main challenge facing graphene device research. Experiments that probe carrier scattering in devices are often indirect, relying on the predictions of a specific model for scattering, such as random charged impurities in the substrate. Here, we describe model-independent, atomic-scale transport measurements that show that scattering at two key defects--surface steps and changes in layer thickness--seriously degrades transport in epitaxial graphene films on SiC. These measurements demonstrate the strong impact of atomic-scale substrate features on graphene performance.

Identifying charge states of molecules with spin-flip spectroscopy.

The charge states of single molecular magnetic chains were manipulated with a scanning tunneling microscope and identified by spin-flip inelastic tunneling spectroscopy. We show that the charged and neutral states have different spin structures and therefore exhibit different features associated with the spin-flip processes in tunneling spectra. The experiment demonstrates a general approach for detecting the charge states at the nanometer scale in a more straightforward manner than using indirect information.

Probing superexchange interaction in molecular magnets by spin-flip spectroscopy and microscopy.

The superexchange mechanism in cobalt phthalocyanine (CoPc) thin films was studied by a low temperature scanning tunneling microscope. The CoPc molecules were found to form one-dimensional antiferromagnetic chains in the film. Collective spin excitations in individual molecular chains were measured with spin-flip associated inelastic electron tunneling spectroscopy. By spatially mapping the spin-flipping channels with submolecular precision, we are able to explicitly identify the specific molecular orbitals that mediate the superexchange interaction between molecules.

High-resolution scanning tunneling spectroscopy of magnetic impurity induced bound states in the superconducting gap of Pb thin films.

Tunneling spectra for individual atoms and dimers of Mn and Cr adsorbed on superconducting Pb thin films were measured by a low temperature scanning tunneling microscope. Multiple-resonance structures within the superconducting gap on the adsorbates were resolved and interpreted as the magnetic impurity-induced bound states associated with different scattering channels. The experiment demonstrates a spectroscopic approach to characterizing the spin states of magnetic structures and exploring the competition between superconductivity and magnetism at the nanometer scale.

An unusual magnetoresistance effect in the heterojunction structure of an ultrathin single-crystal Pb film on silicon substrate.

Superconductor films on semiconductor substrates have drawn much attention recently since the derived superconductor-based electronics have been shown to be promising for future data processing and storage technologies. By growing atomically uniform single-crystal epitaxial Pb films of several nanometers thick on Si wafers to form a sharp superconductor-semiconductor heterojunction, we have obtained an unusual magnetoresistance effect when the Pb film is superconducting. In addition to the large fundamental interest in this effect, the simple structure, and compatibility and scalability with current Si-based semiconductor technology offer a great opportunity for integrating superconducting circuits and detectors in a single chip.

Manipulating the Kondo resonance through quantum size effects.

Manipulating the Kondo effect by quantum confinement has been achieved by placing magnetic molecules on silicon-supported nanostructures. The Kondo resonance of individual manganese phthalocyanine (MnPc) molecules adsorbed on the top of Pb islands was studied by scanning tunneling spectroscopy. Oscillating Kondo temperatures as a function of film thickness were observed and attributed to the formation of the thickness-dependent quantum-well states in the host Pb islands. The present approach provides a technologically feasible way for single spin manipulation by precise thickness control of thin films.