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The strong electron-electron interaction in transition metal dichalcogenides (TMDs) gives rise to phenomena such as strong exciton and trion binding and excitonic condensation, as well as large negative exchange and correlation contributions to the electron energies, resulting in negative electronic compressibility. Here we use angle-resolved photoemission spectroscopy to demonstrate a striking effect of negative electronic compressibility in semiconducting TMD MoS2 on the charge transfer to and from a partial overlayer of monolayer semimetallic WTe2. We track the changes in binding energy of the valence bands of both WTe2 and MoS2 as a function of surface transfer doping with donor (K) and acceptor (F4-TCNQ) species. Donor doping increases the binding energy of the MoS2 valence band, as expected, while counterintuitively reducing the binding energy of the WTe2 valence bands and core levels. The inverse effect is observed for acceptor doping, where a typical reduction in the MoS2 binding energies is accopanied by an unexpected increase in those of WTe2. The observations imply a reversal of the expected charge transfer; donor (acceptor) deposition decreases (increases) the carrier density in the WTe2 adlayer. The charge transfer reversal is a direct consequence of the negative electronic compressibility of the MoS2 surface layer, for which addition (subtraction) of charge leads to attraction (repulsion) of further charge from neighbouring layers. These findings highlight the importance of many-body interactions for the electrons in transition metal dichalcogenides and underscore the potential for exploring strongly correlated quantum states in two-dimensional semiconductors., Comment: 4 pages, 5 figures + supplementary information

We have characterised the submonolayer assembly of C60F48 molecular surface acceptors on the hydrogen terminated (100) diamond surface using scanning tunneling microscopy and X-ray photoelectron spectroscopy, and explored the influence this assembly has on the energy level alignment which governs surface transfer doping. Following deposition, disordered multilayered islands are observed. Annealing to 90$^{\circ} \rm{C}$ causes a transition from dewetting multi-layered islands to a single wetting layer at sufficiently high coverage, accompanied by a change in the energy alignment between the C60F48 and the diamond surface which consequently decreased the carrier density induced by transfer doping by 20%., Comment: 13 pages, 10 figures, preprint

2D topological insulators promise novel approaches towards electronic, spintronic, and quantum device applications. This is owing to unique features of their electronic band structure, in which bulk-boundary correspondences enforces the existence of 1D spin-momentum locked metallic edge states - both helical and chiral - surrounding an electrically insulating bulk. Forty years since the first discoveries of topological phases in condensed matter, the abstract concept of band topology has sprung into realization with several materials now available in which sizable bulk energy gaps - up to a few hundred meV - promise to enable topology for applications even at room-temperature. Further, the possibility of combining 2D TIs in heterostructures with functional materials such as multiferroics, ferromagnets, and superconductors, vastly extends the range of applicability beyond their intrinsic properties. While 2D TIs remain a unique testbed for questions of fundamental condensed matter physics, proposals seek to control the topologically protected bulk or boundary states electrically, or even induce topological phase transitions to engender switching functionality. Induction of superconducting pairing in 2D TIs strives to realize non-Abelian quasiparticles, promising avenues towards fault-tolerant topological quantum computing. This roadmap aims to present a status update of the field, reviewing recent advances and remaining challenges in theoretical understanding, materials synthesis, physical characterization and, ultimately, device perspectives.

Moire superlattices formed in van der Waals heterostructures due to twisting, lattice mismatch and strain present an opportunity for creating novel metamaterials with unique properties not present in the individual layers themselves. Ferroelectricity for example, arises due to broken inversion symmetry in twisted and strained bilayers of 2D semiconductors with stacking domains of alternating out-of-plane polarization. However, understanding the individual contributions of twist and strain to the formation of topological polar nanostructures remains to be established and has proven to be experimentally challenging. Inversion symmetry breaking has been predicted to give rise to an in-plane component of polarization along the domain walls, leading to the formation of a network of topologically non-trivial merons (half-skyrmions) that are Bloch-type for twisted and Neel-type for strained systems. Here we utilise angle-resolved, high-resolution vector piezoresponse force microscopy (PFM) to spatially resolve polarization components and topological polar nanostructures in marginally twisted bilayer WSe2, and provide experimental proof for the existence of topologically non-trivial meron/antimeron structures. We observe both Bloch-type and Neel-type merons, allowing us to differentiate between moire superlattices formed due to twist or heterogeneous strain. This first demonstration of non-trivial real-space topology in a twisted van der Waals heterostructure opens pathways for exploring the connection between twist and topology in engineered nano-devices.

Van der Waals electrode integration is a promising strategy to create near-perfect interfaces between metals and two-dimensional materials, with advantages such as eliminating Fermi-level pinning and reducing contact resistance. However, the lack of a simple, generalizable pick-and-place transfer technology has greatly hampered the wide use of this technique. We demonstrate the pick-and-place transfer of pre-fabricated electrodes from reusable polished hydrogenated diamond substrates without the use of any surface treatments or sacrificial layers. The technique enables transfer of large-scale arbitrary metal electrodes, as demonstrated by successful transfer of eight different elemental metals with work functions ranging from 4.22 to 5.65 eV. The mechanical transfer of metal electrodes from diamond onto van der Waals materials creates atomically smooth interfaces with no interstitial impurities or disorder, as observed with cross-sectional high-resolution transmission electron microscopy and energy-dispersive X-ray spectroscopy. As a demonstration of its device application, we use the diamond-transfer technique to create metal contacts to monolayer transition metal dichalcogenide semiconductors with high-work-function Pd, low-work-function Ti, and semi metal Bi to create n- and p-type field-effect transistors with low Schottky barrier heights. We also extend this technology to other applications such as ambipolar transistor and optoelectronics, paving the way for new device architectures and high-performance devices.

We study quasi-freestanding bilayer graphene on silicon carbide intercalated by calcium. The intercalation, and subsequent changes to the system, were investigated by low-energy electron diffraction, angle-resolved photoemission spectroscopy (ARPES) and density-functional theory (DFT). Calcium is found to intercalate only at the graphene-SiC interface, completely displacing the hydrogen terminating SiC. As a consequence, the system becomes highly n-doped. Comparison to DFT calculations shows that the band dispersion, as determined by ARPES, deviates from the band structure expected for Bernal-stacked bilayer graphene. Instead, the electronic structure closely matches AA-stacked bilayer graphene on Ca-terminated SiC, indicating a spontaneous transition from AB- to AA-stacked bilayer graphene following calcium intercalation of the underlying graphene-SiC interface., Comment: 14 pages, 3 figures

Floquet engineering provides an optical means to manipulate electronic bandstructures, however, carriers excited by the pump field can lead to an effective heating, and can obscure measurement of the band changes. A recent demonstration of the effects of Floquet engineering on a coherent ensemble of excitons in monolayer WS$_2$ proved particularly sensitive to non-adiabatic effects, while still being able to accurately resolve bandstructure changes. Here, we drive an AC-Stark effect in monolayer WS$_2$ using pulses with constant fluence but varying pulse duration (from 25-235~fs). With shorter pump pulses, the corresponding increase in peak intensity introduces additional carriers via two-photon absorption, leading to additional decoherence and peak broadening (which makes it difficult to resolve the AC-Stark shift). We use multidimensional coherent spectroscopy to create a coherent ensemble of excitons in monolayer WS$_2$ and measure the evolution of the coherence throughout the duration of the Floquet pump pulse. Changes to the amplitude of the macroscopic coherence quantifies the additional broadening. At the same time, the evolution of the average phase allows the instantaneous changes to the bandstructure to be quantified, and is not impacted by the additional broadening. This approach to measuring the evolution of Floquet-Bloch states demonstrates a means to quantify effective heating and non-adiabaticity caused by excited carriers, while at the same time resolving the coherent evolution of the bandstructure.

Magnesium intercalated 'quasi-freestanding' bilayer graphene on 6H-SiC(0001) (Mg-QFSBLG) has many favorable properties (e.g., highly n-type doped, relatively stable in ambient conditions). However, intercalation of Mg underneath monolayer graphene is challenging, requiring multiple intercalation steps. Here, we overcome these challenges and subsequently increase the rate of Mg intercalation by laser patterning (ablating) the graphene to form micron-sized discontinuities. We then use low energy electron diffraction to verify Mg-intercalation and conversion to Mg-QFSBLG, and X-ray photoelectron spectroscopy to determine the Mg intercalation rate for patterned and non-patterned samples. By modeling Mg intercalation with the Verhulst equation, we find that the intercalation rate increase for the patterned sample is 4.5$\pm$1.7. Since the edge length of the patterned sample is $\approx$5.2 times that of the non-patterned sample, the model implies that the increased intercalation rate is proportional to the increase in edge length. Moreover, Mg intercalation likely begins at graphene discontinuities in pristine samples (not step edges or flat terraces), where the 2D-like crystal growth of Mg-silicide proceeds. Our laser patterning technique may enable the rapid intercalation of other atomic or molecular species, thereby expanding upon the library of intercalants used to modify the characteristics of graphene, or other 2D materials and heterostructures., Comment: 24 pages, 4 figures

Chalcogen vacancies in transition metal dichalcogenides are widely acknowledged as both donor dopants and as a source of disorder. The electronic structure of sulphur vacancies in MoS2 however is still controversial, with discrepancies in the literature pertaining to the origin of the in-gap features observed via scanning tunneling spectroscopy (STS) on single sulphur vacancies. Here we use a combination of scanning tunnelling microscopy (STM) and STS to study embedded sulphur vacancies in bulk MoS2 crystals. We observe spectroscopic features dispersing in real space and in energy, which we interpret as tip position- and bias-dependent ionization of the sulphur vacancy donor due to tip induced band bending (TIBB). The observations indicate that care must be taken in interpreting defect spectra as reflecting in-gap density of states, and may explain discrepancies in the literature., Comment: 7 pages, 5 figures

Coherent optical manipulation of electronic bandstructures via Floquet Engineering is a promising means to control quantum systems on an ultrafast timescale. However, the ultrafast switching on/off of the driving field comes with questions regarding the limits of validity of the Floquet formalism, which is defined for an infinite periodic drive, and to what extent the transient changes can be driven adibatically. Experimentally addressing these questions has been difficult, in large part due to the absence of an established technique to measure coherent dynamics through the duration of the pulse. Here, using multidimensional coherent spectroscopy we explicitly excite, control, and probe a coherent superposition of excitons in the $K$ and $K^\prime$ valleys in monolayer WS$_2$. With a circularly polarized, red-detuned, pump pulse, the degeneracy of the $K$ and $K^\prime$ excitons can be lifted and the phase of the coherence rotated. We demonstrate phase rotations during the 100 fs driving pulse that exceed $\pi$, and show that this can be described by a combination of the AC-Stark shift of excitons in one valley and Bloch-Siegert shift of excitons in the opposite valley. Despite showing a smooth evolution of the phase that directly follows the intensity envelope of the pump pulse, the process is not perfectly adiabatic. By measuring the magnitude of the macroscopic coherence as it evolves before, during, and after the pump pulse we show that there is additional decoherence caused by power broadening in the presence of the pump. This non-adiabaticity may be a problem for many applications, such as manipulating q-bits in quantum information processing, however these measurements also suggest ways such effects can be minimised or eliminated.

Quantum anomalous Hall (QAH) insulators transport charge without resistance along topologically protected chiral one-dimensional edge states. Yet, in magnetic topological insulators (MTI) to date, topological protection is far from robust, with the zero-magnetic field QAH effect only realised at temperatures an order of magnitude below the N\'eel temperature TN, though small magnetic fields can stabilize QAH effect. Understanding why topological protection breaks down is therefore essential to realising QAH effect at higher temperatures. Here we use a scanning tunnelling microscope to directly map the size of the exchange gap (Eg,ex) and its spatial fluctuation in the QAH insulator 5-layer MnBi$_2$Te$_4$. We observe long-range fluctuations of Eg,ex with values ranging between 0 (gapless) and 70 meV, uncorrelated to individual point defects. We directly image the breakdown of topological protection, showing that the chiral edge state, the hallmark signature of a QAH insulator, hybridizes with extended gapless metallic regions in the bulk. Finally, we unambiguously demonstrate that the gapless regions originate in magnetic disorder, by demonstrating that a small magnetic field restores Eg,ex in these regions, explaining the recovery of topological protection in magnetic fields. Our results indicate that overcoming magnetic disorder is key to exploiting the unique properties of QAH insulators.

Emergent quantum phenomena in two-dimensional van der Waal (vdW) magnets are largely governed by the interplay between the exchange and Coulomb interactions. The ability to tune the Coulomb interaction in such strongly correlated materials enables the precise control of spin-correlated flat-band states, bandgap (Eg) and unconventional magnetism, all of which are crucial for next-generation spintronics and magnonics applications. Here, we demonstrate a giant gate-tunable renormalization of spin-correlated flat-band states and bandgap in magnetic chromium tribromide (CrBr3) monolayers grown on graphene. Our gate-dependent scanning tunneling spectroscopy (STS) studies reveal that the inter-flat-band spacing and bandgap of CrBr3 can be continuously tuned by 120 meV and 240 meV respectively via electrostatic injection of carriers into the hybrid CrBr3/graphene system, equivalent to the modulation of the Cr on-site Coulomb repulsion energy by 500 meV. This can be attributed to the self-screening of CrBr3 arising from the gate-induced carriers injected into CrBr3, which dominates over the opposite trend from the remote screening of the graphene substrate. Precise tuning of the spin-correlated flat-band states and bandgap in 2D magnets via electrostatic modulation of Coulomb interactions not only provides new strategies for optimizing the spin transport channels but also may exert a crucial influence on the exchange energy and spin-wave gap, which could raise the critical temperature for magnetic order., Comment: 21 pages, 4 figures

Strain-induced pseudo magnetic fields offer the possibility of realizing zero magnetic field Quantum Hall effect in graphene, possibly up to room temperature, representing a promising avenue for lossless charge transport applications. Strain engineering on graphene has been achieved via random nanobubbles or artificial nanostructures on the substrate, but the highly localized and non-uniform pseudomagnetic fields can make spectroscopic probes of electronic structure difficult. Heterostructure engineering offers an alternative approach: By stacking graphene on top of another van der Waals material with large lattice mismatch at a desired twist angle, it is possible to generate large strain-induced pseudo magnetic fields uniformly over the entire heterostructure. Here, we report using nano-angle resolved photoemission spectroscopy (nano-ARPES) to probe the electronic bandstructure of a graphene/black phosphorus heterostructure (G/BP). By directly measuring the iso-energy contours of graphene and black phosphorus we determine a twist angle of 20-degrees in our heterostructure. High-resolution nano-ARPES of the graphene bands near the Fermi level reveals the emergence of flat bands located within the Dirac cone. The spacing of the flat bands is consistent with Landau level formation in graphene, and corresponds to a pseudo-field of 11.36 T. Our work provides a new way to study quantum Hall phases induced by strain in 2D materials and heterostructures.

The surface area of Bi2Te3 thin films was increased by introducing nanoscale porosity. Temperature dependent resistivity and magnetotransport measurements were conducted both on as-grown and porous samples (23 and 70 nm). The longitudinal resistivity of the porous samples became more metallic, indicating the increased surface area resulted in transport that was more surface-like. Weak antilocalization (WAL) was present in all samples, and remarkably the phase coherence length doubled in the porous samples. This increase is likely due to the large Fermi velocity of the Dirac surface states. Our results show that the introduction of nanoporosity does not destroy the topological surface states but rather enhances them, making these nanostructured materials promising for low energy electronics, spintronics and thermoelectrics.

A topological quantum field effect transistor (TQFET) uses electric field to switch a material from topological insulator ("on", with conducting edge states) to a conventional insulator ("off"), and can have low subthreshold swing due to strong Rashba spin-orbit interaction. Numerous materials have been proposed, and electric field switching has been demonstrated in ultrathin Na${_3}$Bi. Here we propose a negative capacitance (NC) TQFET which uses a ferroelectric to amplify the electric field and potentially achieve very low switching voltages and energies. Materials challenges for realizing the NC-TQFET are discussed., Comment: Accepted version of paper number 38-2 presented at the 67th Annual IEEE International Electron Devices Meeting (IEDM) on 15 December 2021

Understanding the air-stability of MnBi$_2$Te$_4$ thin films is crucial for the development and long-term operation of electronic devices based around magnetic topological insulators. In the present work, we study MnBi$_2$Te$_4$ thin films upon exposure to atmosphere using a combination of synchrotron-based photoelectron spectroscopy, room temperature electrical transport and atomic force microscopy to determine the oxidation process. After 2 days air exposure a 2 nm thick oxide passivates the surface, corresponding to oxidation of only the top two surface layers, with the underlying layers preserved. This protective oxide layer results in samples that still exhibit metallic conduction even after several days air exposure. Furthermore, the work function decreases from 4.4 eV for pristine MnBi$_2$Te$_4$ to 4.0 eV after the formation of the oxide, along with only a small shift in the core levels indicating minimal doping as a result of air exposure. With the oxide confined to the top surface layers, and the underlying layers preserved, it may be possible to explore new avenues in how to handle, prepare and passivate future MnBi$_2$Te$_4$ devices.

Combining magnetism and nontrivial band topology gives rise to quantum anomalous Hall (QAH) insulators and exotic quantum phases such as the QAH effect where current flows without dissipation along quantized edge states. Inducing magnetic order in topological insulators via proximity to a magnetic material offers a promising pathway towards achieving QAH effect at high temperature for lossless transport applications. One promising architecture involves a sandwich structure comprising two single layers of MnBi2Te4 (a 2D ferromagnetic insulator) with ultra-thin Bi2Te3 in the middle, and is predicted to yield a robust QAH insulator phase with a bandgap well above thermal energy at room temperature (25 meV). Here we demonstrate the growth of a 1SL MnBi2Te4 / 4QL Bi2Te3 /1SL MnBi2Te4 heterostructure via molecular beam epitaxy, and probe the electronic structure using angle resolved photoelectron spectroscopy. We observe strong hexagonally warped massive Dirac Fermions and a bandgap of 75 meV. The magnetic origin of the gap is confirmed by the observation of broken time reversal symmetry and the exchange-Rashba effect, in excellent agreement with density functional theory calculations. These findings provide insights into magnetic proximity effects in topological insulators, that will move lossless transport in topological insulators towards higher temperature., Comment: 24 pages

Inducing long-range magnetic order in three-dimensional topological insulators can gap the Diraclike metallic surface states, leading to exotic new phases such as the quantum anomalous Hall effect or the axion insulator state. These magnetic topological phases can host robust, dissipationless charge and spin currents or unique magnetoelectric behavior, which can be exploited in low-energy electronics and spintronics applications. Although several different strategies have been successfully implemented to realize these states, to date these phenomena have been confined to temperatures below a few Kelvin. In this review, we focus on one strategy, inducing magnetic order in topological insulators by proximity of magnetic materials, which has the capability for room temperature operation, unlocking the potential of magnetic topological phases for applications. We discuss the unique advantages of this strategy, the important physical mechanisms facilitating magnetic proximity effect, and the recent progress to achieve, understand, and harness proximity-coupled magnetic order in topological insulators. We also highlight some emerging new phenomena and applications enabled by proximity coupling of magnetism and topological materials, such as skyrmions and the topological Hall effect, and we conclude with an outlook on remaining challenges and opportunities in the field., Comment: Review article, 30 pages including references, 11 figures

Intrinsic magnetic topological insulators offer low disorder and large magnetic bandgaps for robust magnetic topological phases operating at higher temperatures. By controlling the layer thickness, emergent phenomena such as the Quantum Anomalous Hall (QAH) effect and axion insulator phases have been realised. These observations occur at temperatures significantly lower than the Neel temperature of bulk MnBi2Te4, and measurement of the magnetic energy gap at the Dirac point in ultra-thin MnBi2Te4 has yet to be achieved. Critical to achieving the promise of this system is a direct measurement of the layer-dependent energy gap and verifying whether the gap is magnetic in the QAH phase. Here we utilise temperature dependent angle-resolved photoemission spectroscopy to study epitaxial ultra-thin MnBi2Te4. We directly observe a layer dependent crossover from a 2D ferromagnetic insulator with a bandgap greater than 780 meV in one septuple layer (1 SL) to a QAH insulator with a large energy gap (>100 meV) at 8 K in 3 and 5 SL MnBi2Te4. The QAH gap is confirmed to be magnetic in origin, as it abruptly diminishes with increasing temperature above 8 K. The direct observation of a large magnetic energy gap in the QAH phase of few-SL MnBi2Te4 is promising for further increasing the operating temperature of QAH materials.

We use angle-resolved photoemission spectroscopy to investigate the electronic structure of bilayer graphene at high n-doping and extreme displacement fields, created by intercalating epitaxial monolayer graphene on silicon carbide with magnesium to form quasi-freestanding bilayer graphene on magnesium-terminated silicon carbide. Angle-resolved photoemission spectroscopy reveals that upon magnesium intercalation, the single massless Dirac band of epitaxial monolayer graphene is transformed into the characteristic massive double-band Dirac spectrum of quasi-freestanding bilayer graphene. Analysis of the spectrum using a simple tight binding model indicates that magnesium intercalation results in an n-type doping of 2.1 $\times$ 10$^{14}$ cm$^{-2}$, creates an extremely high displacement field of 2.6 V/nm, opening a considerable gap of 0.36 eV at the Dirac point. This is further confirmed by density-functional theory calculations for quasi-freestanding bilayer graphene on magnesium-terminated silicon carbide, which show a similar doping level, displacement field and bandgap. Finally, magnesium-intercalated samples are surprisingly robust to ambient conditions; no significant changes in the electronic structure are observed after 30 minutes exposure in air., Comment: 46 pages including supporting information, 4 figures in the main paper and 9 figures in the supporting information

The intercalation of epitaxial graphene on SiC(0001) with Ca has been studied extensively, yet precisely where the Ca resides remains elusive. Furthermore, the intercalation of Mg underneath epitaxial graphene on SiC(0001) has not been reported. Here, we use low energy electron diffraction, x-ray photoelectron spectroscopy, secondary electron cut-off photoemission and scanning tunneling microscopy to elucidate the physical and electronic structure of both Ca- and Mg-intercalated epitaxial graphene on 6H-SiC(0001). We find that Ca intercalates underneath the buffer layer and bonds to the Si-terminated SiC surface, breaking the C-Si bonds of the buffer layer i.e. 'freestanding' the buffer layer to form Ca-intercalated quasi-freestanding bilayer graphene (Ca-QFSBLG). The situation is similar for the Mg-intercalation of epitaxial graphene on SiC(0001), where an ordered Mg-terminated reconstruction at the SiC surface and Mg bonds to the Si-terminated SiC surface are formed, resulting in Mg-intercalated quasi-freestanding bilayer graphene (Mg-QFSBLG). Ca-intercalation underneath the buffer layer has not been considered in previous studies of Ca-intercalated epitaxial graphene. Furthermore, we find no evidence that either Ca or Mg intercalates between graphene layers. However, we do find that both Ca-QFSBLG and Mg-QFSBLG exhibit very low workfunctions of 3.68 and 3.78 eV, respectively, indicating high n-type doping. Upon exposure to ambient conditions, we find Ca-QFSBLG degrades rapidly, whereas Mg-QFSBLG remains remarkably stable., Comment: 58 pages, 10 figures, 4 tables. Revised text and figures

Na3Bi has attracted significant interest in both bulk form as a three-dimensional topological Dirac semimetal and in ultra-thin form as a wide-bandgap two-dimensional topological insulator. Its extreme air sensitivity has limited experimental efforts on thin- and ultra-thin films grown via molecular beam epitaxy to ultra-high vacuum environments. Here we demonstrate air-stable Na3Bi thin films passivated with magnesium difluoride (MgF2) or silicon (Si) capping layers. Electrical measurements show that deposition of MgF2 or Si has minimal impact on the transport properties of Na3Bi whilst in ultra-high vacuum. Importantly, the MgF2-passivated Na3Bi films are air-stable and remain metallic for over 100 hours after exposure to air, as compared to near instantaneous degradation when they are unpassivated. Air stability enables transfer of films to a conventional high-magnetic field cryostat, enabling quantum transport measurements which verify that the Dirac semimetal character of Na3Bi films is retained after air exposure.

Layered indium selenides ($In_{2}Se_{3}$) have recently been discovered to host robust out-of-plane and in-plane ferroelectricity in the $\alpha$ and $\beta$' phases, respectively. In this work, we utilise angle-resolved photoelectron spectroscopy to directly measure the electronic bandstructure of $\beta '-In_{2}Se_{3}$, and compare to hybrid density functional theory (DFT) calculations. In agreement with DFT, we find the band structure is highly two-dimensional, with negligible dispersion along the c-axis. Due to n-type doping we are able to observe the conduction band minima, and directly measure the minimum indirect (0.97 eV) and direct (1.46 eV) bandgaps. We find the Fermi surface in the conduction band is characterized by anisotropic electron pockets with sharp in-plane dispersion about the $\overline{M}$ points, yielding effective masses of 0.21 $m_{0}$ along $\overline{KM}$ and 0.33 $m_{0}$ along $\overline{\Gamma M}$. The measured band structure is well supported by hybrid density functional theory calculations. The highly two-dimensional (2D) bandstructure with moderate bandgap and small effective mass suggest that $\beta'-In_{2}Se_{3}$ is a potentially useful new van der Waals semiconductor. This together with its ferroelectricity makes it a viable material for high-mobility ferroelectric-photovoltaic devices, with applications in non-volatile memory switching and renewable energy technologies., Comment: 19 pages, 4 + 1 figures; typos corrected;added references; updated figures & discussion to reflect changes in model

A two-dimensional topological insulator (2DTI) has an insulating bulk and helical spin-polarised edge modes robust to backscattering by non-magnetic disorder. While ballistic transport has been demonstrated in 2DTIs over short distances, larger samples show significant backscattering and a nearly temperature-independent resistance whose origin is unclear. 2DTI edges have shown a spin polarisation, however the degree of helicity is difficult to quantify from spin measurements. Here, we study 2DTI few-layer Na3Bi on insulating Al2O3. A non-local conductance measurement geometry enables sensitive detection of the edge conductance in the topological regime, with an edge mean free path ~100 nm. Magnetic field suppresses spin-flip scattering in the helical edges, resulting in a giant negative magnetoresistance (GNMR), up to 80% at 0.9 T. Comparison to theory indicates >98% of scattering is helical spin scattering significantly exceeding the maximum (67%) expected for a non-helical metal. GNMR, coupled with non-local measurements demonstrating edge conduction, thus provides an unambiguous experimental signature of helical edges that we expect to be generically useful in understanding 2DTIs.

The electric field induced quantum phase transition from topological to conventional insulator has been proposed as the basis of a topological field effect transistor [1-4]. In this scheme an electric field can switch 'on' the ballistic flow of charge and spin along dissipationless edges of the two-dimensional (2D) quantum spin Hall insulator [5-9], and when 'off' is a conventional insulator with no conductive channels. Such as topological transistor is promising for low-energy logic circuits [4], which would necessitate electric field-switched materials with conventional and topological bandgaps much greater than room temperature, significantly greater than proposed to date [6-8]. Topological Dirac semimetals(TDS) are promising systems in which to look for topological field-effect switching, as they lie at the boundary between conventional and topological phases [3,10-16]. Here we use scanning probe microscopy/spectroscopy (STM/STS) and angle-resolved photoelectron spectroscopy (ARPES) to show that mono- and bilayer films of TDS Na3Bi [3,17] are 2D topological insulators with bulk bandgaps >400 meV in the absence of electric field. Upon application of electric field by doping with potassium or by close approach of the STM tip, the bandgap can be completely closed then re-opened with conventional gap greater than 100 meV. The large bandgaps in both the conventional and quantum spin Hall phases, much greater than the thermal energy kT = 25 meV at room temperature, suggest that ultrathin Na3Bi is suitable for room temperature topological transistor operation.

We study the temperature dependence ($77$ K - $475$ K) of the longitudinal resistivity and Hall coefficient of thin films (thickness $20$ nm) of three dimensional topological Dirac semimetal Na$_3$Bi grown via molecular beam epitaxy (MBE). The temperature-dependent Hall coefficient is electron-like at low temperature, but transitions to hole-like transport around $200$ K. We develop a model of a Dirac band with electron-hole asymmetry in Fermi velocity and mobility (assumed proportional to the square of Fermi velocity) which explains well the magnitude and temperature dependence of the Hall resistivity. We find that the hole mobility is about $7$ times larger than the electron mobility. In addition, we find that the electron mobility decreases significantly with increasing temperature, suggesting electron-phonon scattering strongly limits the room temperature mobility., Comment: 12 pages

Large-area thin films of topological Dirac semimetal Na$_3$Bi are grown on amorphous SiO$_2$:Si substrates to realise a field-effect transistor with the doped Si acting as back gate. As-grown films show charge carrier mobilities exceeding 7,000 cm$^2$/Vs and carrier densities below 3 $\times $10$^{18}$ cm$^{-3}$, comparable to the best thin-film Na$_3$Bi. An ambipolar field effect and minimum conductivity are observed, characteristic of Dirac electronic systems. The results are quantitatively understood within a model of disorder-induced charge inhomogeneity in topological Dirac semimetals. Due to the inverted band structure, the hole mobility is significantly larger than the electron mobility in Na$_3$Bi, and when present, these holes dominate the transport properties., Comment: 5 pages, 4 figures; minor corrections and revisions for readability

The close approach of the Fermi energy EF of a Dirac semimetal to the Dirac point ED uncovers new physics such as velocity renormalization,1,2,3 and the Dirac plasma 4,5 at |EF -ED| < kBT, where kBT is the thermal energy. In graphene, substrate disorder drives fluctuations in EF. Three-dimensional topological Dirac semimetals (TDS)6,7 obviate the substrate, and should show reduced EF fluctuations due to better metallic screening and higher dielectric constants. Here we map the potential fluctuations in TDS Na3Bi using a scanning tunneling microscope. The rms potential fluctuations are significantly smaller than room temperature ({\Delta}EF,rms = 4-6 meV = 40-70 K) and comparable to the highest quality graphene on h-BN;8 far smaller than graphene on SiO2,9,10 or the Dirac surface state of a topological insulator.11 Surface Na vacancies produce a novel resonance close to the Dirac point with surprisingly large spatial extent and provides a unique way to tune the surface density of states in a TDS thin-film material., Comment: 25 pages (7 main manuscript), 9 figues (4 main manuscript)

Layered transition metal dichalcogenides (TMDs) are ideal systems for exploring the effects of dimensionality on correlated electronic phases such as charge density wave (CDW) order and superconductivity. In bulk NbSe2 a CDW sets in at TCDW = 33 K and superconductivity sets in at Tc = 7.2 K. Below Tc these electronic states coexist but their microscopic formation mechanisms remain controversial. Here we present an electronic characterization study of a single 2D layer of NbSe2 by means of low temperature scanning tunneling microscopy/spectroscopy (STM/STS), angle-resolved photoemission spectroscopy (ARPES), and electrical transport measurements. We demonstrate that 3x3 CDW order in NbSe2 remains intact in 2D. Superconductivity also still remains in the 2D limit, but its onset temperature is depressed to 1.9 K. Our STS measurements at 5 K reveal a CDW gap of {\Delta} = 4 meV at the Fermi energy, which is accessible via STS due to the removal of bands crossing the Fermi level for a single layer. Our observations are consistent with the simplified (compared to bulk) electronic structure of single-layer NbSe2, thus providing new insight into CDW formation and superconductivity in this model strongly-correlated system., Comment: Nature Physics (2015), DOI:10.1038/nphys3527

We report large negative electron affinity (NEA) on diamond (100) using magnesium adsorption on a previously oxygen-terminated surface. The measured NEA is up to $(-2.01\pm0.05)$ eV, the largest reported negative electron affinity to date. Despite the expected close relationship between the surface chemistry of Mg and Li species on oxygen-terminated diamond, we observe differences in the adsorption properties between the two. Most importantly, a high-temperature annealing step is not required to activate the Mg-adsorbed surface to a state of negative electron affinity. Diamond surfaces prepared by this procedure continue to possess negative electron affinity after exposure to high temperatures, air and even immersion in water., Comment: 7 pages, 5 figures

Magneto-transport measurements were performed on surface conducting hydrogen-terminated diamond (100) hall bars at temperatures between 0.1-5 K in magnetic fields up to 8T., Comment: 2 pages Optoelectronic and Microelectronic Materials & Devices (COMMAD), 2012 Conference

Using microwave-assisted plasma chemical vapour deposition (CVD) a layer of Nitrogen doped ultra-nano-crystalline diamond (N-UNCD) is deposited on top of a non-conducting diamond layer, which itself is situated on a Silicon wafer. This structure is then shaped into Hall-bar devices of various dimensions using optical lithography and dry-etching techniques. The devices' electrical properties are investigated at various temperatures using a cryogen-free dilution refrigerator., Comment: 2 pages Optoelectronic and Microelectronic Materials & Devices (COMMAD), 2012 Conference