Showing papers on "Scanning tunneling spectroscopy published in 2022"

Recent progresses of quantum confinement in graphene quantum dots

Abstract: Graphene quantum dots (GQDs) not only have potential applications on spin qubit, but also serve as essential platforms to study the fundamental properties of Dirac fermions, such as Klein tunneling and Berry phase. By now, the study of quantum confinement in GQDs still attract much attention in condensed matter physics. In this article, we review the experimental progresses on quantum confinement in GQDs mainly by using scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS). Here, the GQDs are divided into Klein GQDs, bound-state GQDs and edge-terminated GQDs according to their different confinement strength. Based on the realization of quasi-bound states in Klein GQDs, external perpendicular magnetic field is utilized as a manipulation approach to trigger and control the novel properties by tuning Berry phase and electron-electron (e-e) interaction. The tip-induced edge-free GQDs can serve as an intuitive mean to explore the broken symmetry states at nanoscale and single-electron accuracy, which are expected to be used in studying physical properties of different two-dimensional materials. Moreover, high-spin magnetic ground states are successfully introduced in edge-terminated GQDs by designing and synthesizing triangulene zigzag nanographenes.

Nonbenzenoid High-Spin Polycyclic Hydrocarbons Generated by Atom Manipulation.

Abstract: We report the on-surface synthesis of a nonbenzenoid triradical through dehydrogenation of truxene (C27H18) on coinage metal and insulator surfaces. Voltage pulses applied via the tip of a combined scanning tunneling microscope/atomic force microscope were used to cleave individual C-H bonds in truxene. The resultant final product truxene-5,10,15-triyl (1) was characterized at the single-molecule scale using a combination of atomic force microscopy, scanning tunneling microscopy, and scanning tunneling spectroscopy. Our analyses show that 1 retains its open-shell quartet ground state, predicted by density functional theory, on a two monolayer-thick NaCl layer on a Cu(111) surface. We image the frontier orbital densities of 1 and confirm that they correspond to spin-split singly occupied molecular orbitals. Through our synthetic strategy, we also isolate two reactive intermediates toward the synthesis of 1, derivatives of fluorenyl radical and indeno[1,2-a]fluorene, with predicted open-shell doublet and triplet ground states, respectively. Our results should have bearings on the synthesis of nonbenzenoid high-spin polycyclic frameworks with magnetism beyond Lieb's theorem.

Manipulation of Spin Polarization in Boron-Substituted Graphene Nanoribbons.

Abstract: The design of magnetic topological states due to spin polarization in an extended π carbon system has great potential in spintronics application. Although magnetic zigzag edges in graphene nanoribbons (GNRs) have been investigated earlier, real-space observation and manipulation of spin polarization in a heteroatom substituted system remains challenging. Here, we investigate a zero-bias peak at a boron site embedded at the center of an armchair-type GNR on a AuSiX/Au(111) surface with a combination of low-temperature scanning tunneling microscopy/spectroscopy and density functional theory calculations. After the tip-induced removal of a Si atom connected to two adjacent boron atoms, a clear Kondo resonance peak appeared and was further split by an applied magnetic field of 12 T. This magnetic state can be relayed along the longitudinal axis of the GNR by sequential removal of Si atoms.

Visualization of defect induced in-gap states in monolayer MoS2

Abstract: Abstract Atomic-scale intrinsic defects play a key role in controlling functional electronic properties of two-dimensional (2D) materials. Here, we present a low-temperature scanning–tunneling microscopy and spectroscopy investigation of a common point-defect in monolayer molybdenum disulfide (MoS 2 ). We employ a sample preparation method in which the film surface is never exposed to air so that the native dangling bonds surrounding the defects in the film are preserved. Molybdenum vacancies are identified by their three characteristic in-gap resonances by combining scanning–tunneling measurements with parallel Green’s function-based theoretical modeling. The relative energy shifts between the various in-gap states allow us to identify a relative charge difference between two of the observed vacancies. The role of the substrate on the band structure of the defective MoS 2 monolayer is unveiled. Our study highlights the effects of the substrate on the in-gap states of common defects found in MoS 2 providing a pathway in designing and optimizing 2D materials for electronic applications.

Synthesis and characterization of peri-heptacene on a metallic surface.

Abstract: The synthesis of long n-peri-acenes (n-PAs) is challenging as a result of their inherent open-shell radical character, which arises from the presence of parallel zigzag edges beyond a certain n value. They are considered as π-electron model systems to study magnetism in graphene nanostructures; being potential candidates in the fabrication of optoelectronic and spintronic devices. Here, we report the on-surface formation of the largest pristine member of the n-PA family, i.e. peri-heptacene (n = 7, 7-PA), obtained on an Au(111) substrate under ultra-high vacuum conditions. Our high-resolution scanning tunneling microscopy investigations, complemented by theoretical simulations, provide insight into the chemical structure of this previously elusive compound. In addition, scanning tunneling spectroscopy reveals the antiferromagnetic open-shell singlet ground state of 7-PA, exhibiting singlet-triplet spin-flip inelastic excitations with an effective exchange coupling (Jeff) of 49 meV.

Spatial variation of geometry, binding, and electronic properties in the moiré superstructure of MoS2 on Au(111)

Abstract: The lattice mismatch between a monolayer of MoS2 and its Au(111) substrate induces a moiré superstructure. The local variation of the registry between sulfur and gold atoms at the interface leads to a periodic pattern of strongly and weakly interacting regions. In consequence, also the electronic bands show a spatial variation. We use scanning tunneling microscopy and spectroscopy (STM/STS), x-ray photoelectron spectroscopy (XPS) and x-ray standing wave (XSW) for a determination of the geometric and electronic structure. The experimental results are corroborated by density functional theory. We obtain the geometric structure of the supercell with high precision, identify the fraction of interfacial atoms that are strongly interacting with the substrate, and analyze the variation of the electronic structure in dependence of the location within the moiré unit cell and the nature of the band.

Twisted bilayer zigzag-graphene nanoribbon junctions with tunable edge states

Abstract: Stacking two-dimensional layered materials such as graphene and transitional metal dichalcogenides with nonzero interlayer twist angles has recently become attractive because of the emergence of novel physical properties. Stacking of one-dimensional nanomaterials offers the lateral stacking offset as an additional parameter for modulating the resulting material properties. Here, we report that the edge states of twisted bilayer zigzag graphene nanoribbons (TBZGNRs) can be tuned with both the twist angle and the stacking offset. Strong edge state variations in the stacking region are first revealed by density functional theory (DFT) calculations. We construct and characterize twisted bilayer zigzag graphene nanoribbon (TBZGNR) systems on a Au(111) surface using scanning tunneling microscopy. A detailed analysis of three prototypical orthogonal TBZGNR junctions exhibiting different stacking offsets by means of scanning tunneling spectroscopy reveals emergent near-zero-energy states. From a comparison with DFT calculations, we conclude that the emergent edge states originate from the formation of flat bands whose energy and spin degeneracy are highly tunable with the stacking offset. Our work highlights fundamental differences between 2D and 1D twistronics and spurs further investigation of twisted one-dimensional systems.

Origin of Asymmetric Splitting of Kondo Peak in Spin-Polarized Scanning Tunneling Spectroscopy: Insights from First-Principles-Based Simulations.

Abstract: The spin-polarized scanning tunneling microscope (SP-STM) has served as a versatile tool for probing and manipulating the spintronic properties of atomic and molecular devices with high precision. The interplay between the local spin state and its surrounding magnetic environment significantly affects the transport behavior of the device. Particularly, in the contact regime, the strong hybridization between the SP-STM tip and the magnetic atom or molecule could give rise to unconventional Kondo resonance signatures in the differential conductance (dI/dV) spectra. This poses challenges for the simulation of a realistic tip control process. By combining the density functional theory and the hierarchical equations of motion methods, we achieve first-principles-based simulation of the control of a Ni-tip/Co/Cu(100) junction in both the tunneling and contact regimes. The calculated dI/dV spectra reproduce faithfully the experimental data. A cotunneling mechanism is proposed to elucidate the physical origin of the observed unconventional Kondo signatures.

Microwave-Frequency Scanning Gate Microscopy of a Si/SiGe Double Quantum Dot.

Abstract: Conventional transport methods provide quantitative information on spin, orbital, and valley states in quantum dots but lack spatial resolution. Scanning tunneling microscopy, on the other hand, provides exquisite spatial resolution at the expense of speed. Working to combine the spatial resolution and energy sensitivity of scanning probe microscopy with the speed of microwave measurements, we couple a metallic tip to a Si/SiGe double quantum dot (DQD) that is integrated with a charge detector. We first demonstrate that the dc-biased tip can be used to change the occupancy of the DQD. We then apply microwaves through the tip to drive photon-assisted tunneling (PAT). We infer the DQD level diagram from the frequency and detuning dependence of the tunneling resonances. These measurements allow the resolution of ∼65 μeV excited states, an energy consistent with valley splittings in Si/SiGe. This work demonstrates the feasibility of scanning gate experiments with Si/SiGe devices.

Observation of a van Hove singularity of a surface Fermi arc with prominent coupling to phonons in a Weyl semimetal

Abstract: A van der Waals coupled Weyl semimetal ${\mathrm{NbIrTe}}_{4}$ is investigated by combining scanning tunneling microscopy/spectroscopy and first-principles calculations. We observe a sharp peak in the tunneling conductance near the Fermi energy (${E}_{F}$). Comparison with calculations indicates that the peak originates from a van Hove singularity (vHs) associated with a Lifshitz transition of the surface Fermi-arc state. Interestingly, our tunneling spectroscopy also shows signatures of strong electron-boson coupling. This is potentially due to an anomalously enhanced charge susceptibility coming from the near-${E}_{F}$ vHs formation.

Controlling Andreev Bound States with the Magnetic Vector Potential

Abstract: Tunneling spectroscopy measurements are often used to probe the energy spectrum of Andreev bound states (ABSs) in semiconductor-superconductor hybrids. Recently, this spectroscopy technique has been incorporated into planar Josephson junctions (JJs) formed in two-dimensional electron gases, a potential platform to engineer phase-controlled topological superconductivity. Here, we perform ABS spectroscopy at the two ends of planar JJs and study the effects of the magnetic vector potential on the ABS spectrum. We show that the local superconducting phase difference arising from the vector potential is equal in magnitude and opposite in sign at the two ends, in agreement with a model that assumes localized ABSs near the tunnel barriers. Complemented with microscopic simulations, our experiments demonstrate that the local phase difference can be used to estimate the relative position of localized ABSs separated by a few hundred nanometers.

Combining electron spin resonance spectroscopy with scanning tunneling microscopy at high magnetic fields

Abstract: The continuous increase in storage densities and the desire for quantum memories and computers push the limits of magnetic characterization techniques. Ultimately, a tool that is capable of coherently manipulating and detecting individual quantum spins is needed. Scanning tunneling microscopy (STM) is the only technique that unites the prerequisites of high spatial and energy resolution, low temperature, and high magnetic fields to achieve this goal. Limitations in the available frequency range for electron spin resonance STM (ESR-STM) mean that many instruments operate in the thermal noise regime. We resolve challenges in signal delivery to extend the operational frequency range of ESR-STM by more than a factor of two and up to 100 GHz, making the Zeeman energy the dominant energy scale at achievable cryogenic temperatures of a few hundred millikelvin. We present a general method for augmenting existing instruments into ESR-STM to investigate spin dynamics in the high-field limit. We demonstrate the performance of the instrument by analyzing inelastic tunneling in a junction driven by a microwave signal and provide proof of principle measurements for ESR-STM.

Structural and superconducting properties of ultrathin Ir films on Nb(110)

Abstract: The ongoing quest for unambiguous signatures of topological superconductivity and Majorana modes in magnet-superconductor hybrid systems creates a high demand for suitable superconducting substrates. Materials that incorporate $s$-wave superconductivity with a wide energy gap, large spin-orbit coupling, and high surface quality, which enable the atom-by-atom construction of magnetic nanostructures using the tip of a scanning tunneling microscope, are particularly desired. Since single materials rarely fulfill all these requirements, we propose and demonstrate the growth of thin films of a high-Z metal, Ir, on a surface of the elemental superconductor with the largest energy gap, Nb. We find a strained Ir(110)/Nb(110)-oriented superlattice for thin films of one to two atomic layers, which transitions to a compressed Ir(111) surface for thick films of ten atomic layers. Using tunneling spectroscopy, we observe proximity-induced superconductivity in the latter Ir(111) film with a hard gap $\mathrm{\ensuremath{\Delta}}$ that is $85.3%$ of that of bare Nb(110).

Direct observation of the Mottness and p–d orbital hybridization in the epitaxial monolayer α-RuCl₃

Abstract: α-RuCl3, a promising material to accomplish the Kitaev honeycomb model, has attracted enormous interest recently. Mottness and p-d bonds play vital roles in generating Kitaev interactions and underpinning the potential exotic states of quantum magnets, and the van der Waals monolayer is considered to be a better platform to approach a two-dimensional Kitaev model than the bulk. Here, we worked out the growth art of an α-RuCl3 monolayer on a graphite substrate and studied its electronic structure, particularly the delicate orbital occupations, through scanning tunneling microscopy and spectroscopy. An in-plane lattice expansion of 2.67 ± 0.83% is observed and the pronounced t2g-pπ and eg-pσ hybridization are visualized. The Mott nature is unveiled by an ∼0.6 eV full gap at the Fermi level located inside the t2g-pπ manifold which is further verified by the density functional theory calculations. The monolayer phase of α-RuCl3 fulfills the a priori criteria of recent theoretical predictions of tuning the relevant properties in this material and provides a novel platform to explore the Kitaev physics.

Low-Dimensional Porous Carbon Networks Using Single-/Triple-Coupling Polycyclic Hydrocarbon Precursors.

Abstract: Polycyclic hydrocarbons (PHs) share the same hexagonal structure of sp2 carbons as graphene but possess an energy gap due to quantum confinement effect. PHs can be synthesized by a bottom-up strategy starting from small building blocks covalently bonded into large 2D organic sheets. Further investigation of the role of the covalent bonding/coupling ways on their electronic properties is needed. Here, we demonstrate a surface-mediated synthesis of hexa-peri-hexabenzocoronene (HBC) and its extended HBC oligomers (dimers, trimers, and tetramers) via single- and triple-coupling ways and reveal the implication of different covalent bonding on their electronic properties. High-resolution low-temperature scanning tunneling microscopy and noncontact atomic force microscopy are employed to in situ determine the atomic structures of as-synthesized HBC oligomers. Scanning tunneling spectroscopy measurements show that the length extension of HBC oligomers narrows the energy gap between highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO). Furthermore, the energy gaps of triple-coupling HBC oligomers are smaller and decrease more significantly than that of the single-coupling ones. We hypothesize that the triple coupling promotes a more effective delocalization of π-electrons than the single coupling, according to density functional theory calculations. We also demonstrate that the HBC oligomers can further extend across the substrate steps to achieve conjugated polymers and large-area porous carbon networks.

Local Density of States Modulated by Strain in Marginally Twisted Bilayer Graphene

Abstract: In marginally twisted bilayer graphene, the Moiré pattern consists of the maximized AB (BA) stacking regions, minimized AA stacking regions and triangular networks of domain walls. Here we realize the strain-modulated electronic structures of marginally twisted bilayer graphene by scanning tunneling microscopy/spectroscopy and density functional theory (DFT) calculations. The experimental data show four peaks near the Fermi energy at the AA regions. DFT calculations indicate that the two new peaks closer to the Fermi level may originate from the intrinsic heterostrain and the electric field implemented by back gate is likely to account for the observed shift of the four peaks. Furthermore, the dI/dV map across Moiré patterns with different strain strengths exhibits a distinct appearance of the helical edge states.

Tunneling Spectroscopy of Two-Dimensional Materials Based on Via Contacts.

Abstract: We introduce a novel planar tunneling architecture for van der Waals heterostructures based on via contacts, namely, metallic contacts embedded into through-holes in hexagonal boron nitride (hBN). We use the via-based tunneling method to study the single-particle density of states of two different two-dimensional (2D) materials, NbSe2 and graphene. In NbSe2 devices, we characterize the barrier strength and interface disorder for barrier thicknesses of 0, 1, and 2 layers of hBN and study the dependence on the tunnel-contact area down to (44 ± 14)2 nm2. For 0-layer hBN devices, we demonstrate a crossover from diffusive to point contacts in the small-contact-area limit. In graphene, we show that reducing the tunnel barrier thickness and area can suppress effects due to phonon-assisted tunneling and defects in the hBN barrier. This via-based architecture overcomes limitations of other planar tunneling designs and produces high-quality, ultraclean tunneling structures from a variety of 2D materials.

Giant g-factor in Self-Intercalated 2D TaS2.

Abstract: Central to the application of spintronic devices is the ability to manipulate spins by electric and magnetic fields, which relies on a large Landé g-factor. The self-intercalation of layered transitional metal dichalcogenides with native metal atoms can serve as a new strategy to enhance the g-factor by inducing ferromagnetic instability in the system via interlayer charge transfer. Here, scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS) are performed to extract the g-factor and characterize the electronic structure of the self-intercalated phase of 2H-TaS2 . In Ta7 S12 , a sharp density of states (DOS) peak due to the Ta intercalant appears at the Fermi level, which satisfies the Stoner criteria for spontaneous ferromagnetism, leading to spin split states. The DOS peak shows sensitivity to magnetic field up to 1.85 mV T-1 , equivalent to an effective g-factor of ≈77. This work establishes self-intercalation as an approach for tuning the g-factor.

On-surface synthesis and characterization of nitrogen-doped covalent-organic frameworks on Ag(111) substrate.

Abstract: Atomically precise fabrication of covalent-organic frameworks with well-defined heteroatom-dopant sites and further understanding of their electronic properties at the atomic level remain a challenge. Herein, we demonstrate the bottom-up synthesis of well-organized covalent-organic frameworks doped by nitrogen atoms on an Ag(111) substrate. Using high-resolution scanning tunneling microscopy and non-contact atomic force microscopy, the atomic structures of the intermediate metal-organic frameworks and the final covalent-organic frameworks are clearly identified. Scanning tunneling spectroscopy characterization reveals that the electronic bandgap of the as-formed N-doped covalent-organic framework is 2.45 eV, in qualitative agreement with the theoretical calculations. The calculated band structure together with the projected density of states analysis clearly unveils that the incorporation of nitrogen atoms into the covalent-organic framework backbone will remarkably tune the bandgap owing to the fact that the foreign nitrogen atom has one more electron than the carbon atom. Such covalent-organic frameworks may offer an atomic-scale understanding of the local electronic structure of heteroatom-doped covalent-organic frameworks and hold great promise for all relevant wide bandgap semiconductor technologies, for example, electronics, photonics, high-power and high-frequency devices, and solar energy conversion.

Defect-assisted tunneling spectroscopy of electronic band structure in twisted bilayer graphene/hexagonal boron nitride moiré superlattices

Abstract: We report the demonstration of defect-assisted tunneling spectroscopy of the electronic band structure in twisted bilayer graphene (tBLG)/hexagonal boron nitride ( h-BN) moiré superlattices in which the moiré period between the two graphene layers is close to that between the graphene and h-BN layers. We measured both the in-plane and vertical carrier transport in the tBLG/ h-BN van der Waals (vdW) tunneling device. The moiré periods were determined from the in-plane carrier transport measurements. The observed vertical tunneling transport characteristics indicated that resonant tunneling occurs from the graphite electrode to tBLG through localized defect states in the h-BN tunnel barrier. We observed multiple defect-assisted resonant tunneling trajectories, from which we derived the density of states (DOS) for tBLG. The obtained DOS has broad flatband features, in qualitative agreement with the theoretical predictions. Furthermore, we obtained three types of DOS, suggesting that we probed local band structures corresponding to AA, AB/BA, and domain wall sites in tBLG. Thus, defect-assisted tunneling spectroscopy has potential as a tool to determine the local band structures in twisted 2D vdW materials.

Field-Emission Resonances in Thin Metallic Films: Nonexponential Decrease of the Tunneling Current as a Function of the Sample-to-Tip Distance

Abstract: Field-emission resonances (FERs) for two-dimensional Pb(111) islands grown on Si(111)7×7 surfaces were studied by low-temperature scanning tunneling microscopy and spectroscopy (STM/STS) in a broad range of tunneling conditions with both an active and disabled feedback loop. These FERs exist at quantized sample-to-tip distances Zn above the sample surface, where n is the serial number of the FER state. By recording the trajectory of the STM tip during ramping of the bias voltage U (while keeping the tunneling current I fixed), we obtain the set of the Zn values corresponding to local maxima in the derived dZ/dU(U) spectra. This way, the continuous evolution of Zn as a function of U for all FERs was investigated by STS experiments with an active feedback loop for different I. Complementing these measurements by current–distance spectroscopy at a fixed U, we could construct a 4-dimensional I–U–Z–dZ/dU diagram that allows us to investigate the geometric localization of the FERs above the surface. We demonstrate (i) that the difference δZn = Zn+1 – Zn between neighboring FER lines in the Z–U diagram is independent of n for higher resonances; (ii) that the δZn value decreases as U increases; (iii) that the quantized FER states lead to the periodic variations of ln I as a function of Z with periodicity δZ; and (iv) that the periodic variations in the ln I–Z spectra allow an estimation of the absolute height of the tip above the sample surface. Our findings contribute to a deeper understanding on how the FER states affect various types of tunneling spectroscopy experiments and how they lead to a nonexponential decay of the tunneling current as a function of Z at high bias voltages in the regime of quantized electron emission.

Advances in bismuth-based topological quantum materials by scanning tunneling microscopy

Abstract: In recent years, topological quantum materials (TQMs) have attracted intensive attention in the area of condensed matter physics due to their novel topologies and their promising applications in quantum computing, spin electronics and next-generation integrated circuits. Scanning tunneling microscopy/spectroscopy (STM/STS) is regarded as a powerful technique to characterize the local density of states with atomic resolution, which is ideally suited to the measurement of the bulk-boundary correspondence of TQMs. In this review, using STM/STS, we focus on recent research on bismuth-based TQMs, including quantum-spin Hall insulators, 3D weak topological insulators (TIs), high-order TIs, topological Dirac semi-metals and dual TIs. Efficient methods for the modulation of the topological properties of the TQMs are introduced, such as interlayer interaction, thickness variation and local electric field perturbation. Finally, the challenges and prospects for this field of study are discussed.

Unveiling the Decisive Factor for the Sharp Transition in the Scanning Tunneling Spectroscopy of a Single Nickelocene Molecule.

Abstract: Scanning tunneling microscopy (STM) has been utilized to realize the precise measurement and control of local spin states. Experiments have demonstrated that when a nickelocene (Nc) molecule is attached to the apex of an STM tip, the dI/dV spectra exhibit a sharp or a smooth transition when the tip is displaced toward the substrate. However, what leads to the two distinct types of transitions remains unclear, and more intriguingly, the physical origin of the abrupt change in the line shape of dI/dV spectra remains unclear. To clarify these intriguing issues, we perform first-principles-based simulations on the STM tip control process for the Cu tip/Nc/Cu(100) junction. In particular, we find that the suddenly enhanced hybridization between the d orbitals on the Ni ion and the metallic bands in the substrate leads to Kondo correlation overwhelming spin excitation, which is the main cause of the sharp transition in the dI/dV spectra observed experimentally.

Defects, band bending and ionization rings in MoS₂

Abstract: 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 MoS2however 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 and STS to study embedded sulphur vacancies in bulk MoS2crystals. 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. 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.

Tip-Mediated Bandgap Tuning for Monolayer Transition Metal Dichalcogenides.

Abstract: Monolayer transition metal dichalcogenides offer an appropriate platform for developing advanced electronics beyond graphene. Similar to two-dimensional molecular frameworks, the electronic properties of such monolayers can be sensitive to perturbations from the surroundings; the implied tunability of electronic structure is of great interest. Using scanning tunneling microscopy/spectroscopy, we demonstrated a bandgap engineering technique in two monolayer materials, MoS2 and PtTe2, with the tunneling current as a control parameter. The bandgap of monolayer MoS2 decreases logarithmically by the increasing tunneling current, indicating an electric-field-induced gap renormalization effect. Monolayer PtTe2, by contrast, exhibits a much stronger gap reduction, and a reversible semiconductor-to-metal transition occurs at a moderate tunneling current. This unusual switching behavior of monolayer PtTe2, not seen in bulk semimetallic PtTe2, can be attributed to its surface electronic structure that can readily couple to the tunneling tip, as demonstrated by theoretical calculations.

Local density of states and particle entanglement in topological quantum fluids

Abstract: The understanding of particle entanglement is an important goal in the studies of correlated quantum matter. The widely used method of scanning tunneling spectroscopy---which measures the local density of states (LDOS) of a many-body system by injecting or removing an electron from it---is expected to be sensitive to particle entanglement. In this paper, we systematically investigate the relation between the particle entanglement spectrum (PES) and the LDOS of fractional quantum Hall (FQH) states, the paradigmatic strongly correlated phases of electrons with topological order. Using exact diagonalization, we show that the counting of levels in both the LDOS and PES in the Jain sequence of FQH states can be predicted from the composite fermion theory. We point out the differences between LDOS and PES characterization of the bulk quasihole excitations, and we discuss the conditions under which the LDOS counting can be mapped to that of PES. Our results affirm that tunneling spectroscopy is a sensitive tool for identifying the nature of FQH states.

Surface Confined Hydrogenation of Graphene Nanoribbons

Abstract: On-surface synthesis with designer precursor molecules is considered an effective method for preparing graphene nanoribbons (GNRs) of well-defined widths and with tunable electronic properties. Recent reports have shown that the band gap of ribbons doped with heteroatoms (such as boron, nitrogen, and sulfur) remains unchanged in magnitude in most cases. Nevertheless, theory predicts that a tunable band gap may be engineered by hydrogenation, but experimental evidence for this is so far lacking. Herein, surface-confined hydrogenation studies of 7-armchair graphene nanoribbons (7-AGNRs) grown on Au(111) surfaces, in an ultrahigh vacuum environment, are reported. GNRs are first prepared, then hydrogenated by exposure to activated hydrogen atoms. High resolution electron energy loss spectroscopy (HREELS) and scanning tunneling microscopy (STM) images reveal a self-limited hydrogenation process. By means of a combination of bond-resolved scanning tunneling microscopy (BRSTM) imaging and tip-induced site-specific dehydrogenation, the hydrogenation mechanism is studied in detail, and density-functional theory (DFT) calculation methods are used to complement the experimental findings. In all cases, the results demonstrate the successful modification of the electronic properties of the GNR/Au(111) system by edge and basal-plane hydrogenation, and a mechanism for the hydrogenation process is proposed.

Superconducting dome by tuning through a van Hove singularity in a two-dimensional metal

Abstract: Abstract Chemical substitution is a promising route for the exploration of a rich variety of doping- and/or disorder-dependent collective phenomena in low-dimensional quantum materials. Here we show that transition metal dichalcogenide alloys are ideal platforms to this purpose. In particular, we demonstrate the emergence of superconductivity in the otherwise metallic single-layer TaSe 2 by minute electron doping provided by substitutional W atoms. We investigate the temperature and magnetic field dependence of the superconducting state of Ta 1-δ W δ Se 2 with electron doping ( δ ) using variable temperature (0.34–4.2 K) scanning tunneling spectroscopy (STS). We unveil the emergence of a superconducting dome spanning 0.003 < δ < 0.03 with a maximized critical temperature of 0.9 K, a significant increase from that of bulk TaSe 2 ( T C = 0.14 K). Superconductivity emerges from an increase of the density of states (DOS) as the Fermi surface approaches a van Hove singularity due to doping. Once the singularity is reached, however, the DOS decreases with δ , which gradually weakens the superconducting state, thus shaping the superconducting dome. Lastly, our doping-dependent measurements suggest the development of a Coulomb glass phase triggered by disorder due to W dopants.