Showing papers on "Scanning tunneling spectroscopy published in 2020"
TL;DR: In this article, the tunneling conductance of vortex bound states on FeTe0.55Se0.45 superconductors was studied using variable-tunnel-coupled scanning tunneling spectroscopy.
Abstract: Majorana zero modes (MZMs) are spatially localized, zero-energy fractional quasiparticles with non-Abelian braiding statistics that hold promise for topological quantum computing. Owing to the particle-antiparticle equivalence, MZMs exhibit quantized conductance at low temperature. By using variable-tunnel–coupled scanning tunneling spectroscopy, we studied tunneling conductance of vortex bound states on FeTe0.55Se0.45 superconductors. We report observations of conductance plateaus as a function of tunnel coupling for zero-energy vortex bound states with values close to or even reaching the 2e2/h quantum conductance (where e is the electron charge and h is Planck’s constant). By contrast, no plateaus were observed on either finite energy vortex bound states or in the continuum of electronic states outside the superconducting gap. This behavior of the zero-mode conductance supports the existence of MZMs in FeTe0.55Se0.45.
134 citations
TL;DR: It is demonstrated that π paramagnetism of high-spin graphene flakes can survive on surfaces, opening the door to study the quantum behavior of interacting π spins in graphene systems.
Abstract: Graphene can develop large magnetic moments in custom-crafted open-shell nanostructures such as triangulene, a triangular piece of graphene with zigzag edges. Current methods of engineering graphene nanosystems on surfaces succeeded in producing atomically precise open-shell structures, but demonstration of their net spin remains elusive to date. Here, we fabricate triangulenelike graphene systems and demonstrate that they possess a spin S=1 ground state. Scanning tunneling spectroscopy identifies the fingerprint of an underscreened S=1 Kondo state on these flakes at low temperatures, signaling the dominant ferromagnetic interactions between two spins. Combined with simulations based on the meanfield Hubbard model, we show that this S=1 π paramagnetism is robust and can be turned into an S=1/2 state by additional H atoms attached to the radical sites. Our results demonstrate that π paramagnetism of high-spin graphene flakes can survive on surfaces, opening the door to study the quantum behavior of interacting π spins in graphene systems.
103 citations
TL;DR: In this article, a symmetric superlattice of zero-energy modes is proposed to induce metallicity in GNRs by inserting symmetric sublattices into otherwise semiconducting GNRs.
Abstract: The design and fabrication of robust metallic states in graphene nanoribbons (GNRs) are challenging because lateral quantum confinement and many-electron interactions induce electronic band gaps when graphene is patterned at nanometer length scales. Recent developments in bottom-up synthesis have enabled the design and characterization of atomically precise GNRs, but strategies for realizing GNR metallicity have been elusive. Here we demonstrate a general technique for inducing metallicity in GNRs by inserting a symmetric superlattice of zero-energy modes into otherwise semiconducting GNRs. We verify the resulting metallicity using scanning tunneling spectroscopy as well as first-principles density-functional theory and tight-binding calculations. Our results reveal that the metallic bandwidth in GNRs can be tuned over a wide range by controlling the overlap of zero-mode wave functions through intentional sublattice symmetry breaking.
93 citations
TL;DR: The magnetic and electronic properties of CrSBr are reported, an air-stable vdW antiferromagnetic semiconductor that readily cleaves perpendicular to the stacking axis, leading to a large negative magnetoresistance response that is unique amongvdW materials.
Abstract: The recent discovery of magnetism within the family of exfoliatable van der Waals (vdW) compounds has attracted considerable interest in these materials for both fundamental research and technological applications. However, current vdW magnets are limited by their extreme sensitivity to air, low ordering temperatures, and poor charge transport properties. Here the magnetic and electronic properties of CrSBr are reported, an air-stable vdW antiferromagnetic semiconductor that readily cleaves perpendicular to the stacking axis. Below its Neel temperature, TN = 132 ± 1 K, CrSBr adopts an A-type antiferromagnetic structure with each individual layer ferromagnetically ordered internally and the layers coupled antiferromagnetically along the stacking direction. Scanning tunneling spectroscopy and photoluminescence (PL) reveal that the electronic gap is ΔE = 1.5 ± 0.2 eV with a corresponding PL peak centered at 1.25 ± 0.07 eV. Using magnetotransport measurements, strong coupling between magnetic order and transport properties in CrSBr is demonstrated, leading to a large negative magnetoresistance response that is unique among vdW materials. These findings establish CrSBr as a promising material platform for increasing the applicability of vdW magnets to the field of spin-based electronics.
73 citations
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TL;DR: In this paper, the magnetic and electronic properties of CrSBr, an air-stable van der Waals (vdW) antiferromagnetic semiconductor that readily cleaves perpendicular to the stacking axis, were reported.
Abstract: The recent discovery of magnetism within the family of exfoliatable van der Waals (vdW) compounds has attracted considerable interest in these materials for both fundamental research and technological applications. However current vdW magnets are limited by their extreme sensitivity to air, low ordering temperatures, and poor charge transport properties. Here we report the magnetic and electronic properties of CrSBr, an air-stable vdW antiferromagnetic semiconductor that readily cleaves perpendicular to the stacking axis. Below its Neel temperature, $T_N = 132 \pm 1$ K, CrSBr adopts an A-type antiferromagnetic structure with each individual layer ferromagnetically ordered internally and the layers coupled antiferromagnetically along the stacking direction. Scanning tunneling spectroscopy and photoluminescence (PL) reveal that the electronic gap is $\Delta_E = 1.5 \pm 0.2$ eV with a corresponding PL peak centered at $1.25 \pm 0.07$ eV. Using magnetotransport measurements, we demonstrate strong coupling between magnetic order and transport properties in CrSBr, leading to a large negative magnetoresistance response that is unique amongst vdW materials. These findings establish CrSBr as a promising material platform for increasing the applicability of vdW magnets to the field of spin-based electronics.
72 citations
TL;DR: The on-surface generation of the longest acene obtained so far: Dodecacene is presented and it is observed that, after a progressive closing of the gap and a stabilization to about 1 eV at the length of decacene and undecacen, the energy gap of dodecacenes unexpectedly increases to 1.4 eV.
Abstract: The acene series represents a model system to investigate the intriguing electronic properties of extended π-electron structures in the one-dimensional limit, which are important for applications in electronics and spintronics and for the fundamental understanding of electronic transport. Here, we present the on-surface generation of the longest acene obtained so far: dodecacene. Scanning tunneling spectroscopy gives access to the energy position and spatial distribution of its electronic states on the Au(111) surface. We observe that, after a progressive closing of the gap and a stabilization to about 1 eV at the length of decacene and undecacene, the energy gap of dodecacene unexpectedly increases to 1.4 eV. Considering the acene series as an exemplary general case, we discuss the evolution with length of the single tunneling resonances in comparison with ionization energy, electronic affinity, and optical gap.
69 citations
TL;DR: In this paper, on-surface synthesis and a proof-of-principle experimental study of magnetism in covalently bonded triangulene dimers are presented.
Abstract: Triangular zigzag nanographenes, such as triangulene and its pi-extended homologues, have received widespread attention as organic nanomagnets for molecular spintronics, and may serve as building blocks for high-spin networks with long-range magnetic order - of immense fundamental and technological relevance. As a first step toward these lines, we present the on-surface synthesis and a proof-of-principle experimental study of magnetism in covalently bonded triangulene dimers. On-surface reactions of rationally-designed precursor molecules on Au(111) lead to the selective formation of triangulene dimers in which the triangulene units are either directly connected through their minority sublattice atoms, or are separated via a 1,4-phenylene spacer. The chemical structures of the dimers have been characterized by bond-resolved scanning tunneling microscopy. Scanning tunneling spectroscopy and inelastic electron tunneling spectroscopy measurements reveal collective singlet-triplet spin excitations in the dimers, demonstrating efficient inter-triangulene magnetic coupling.
68 citations
TL;DR: In this article, a spin state was detected in electrical transport measurements through boron-substituted nanoribbons suspended between the tip and the sample of a scanning tunneling microscope.
Abstract: Graphene nanoribbons (GNRs), low-dimensional platforms for carbon-based electronics, show the promising perspective to also incorporate spin polarization in their conjugated electron system. However, magnetism in GNRs is generally associated with localized states around zigzag edges, difficult to fabricate and with high reactivity. Here we demonstrate that magnetism can also be induced away from physical GNR zigzag edges through atomically precise engineering topological defects in its interior. A pair of substitutional boron atoms inserted in the carbon backbone breaks the conjugation of their topological bands and builds two spin-polarized boundary states around them. The spin state was detected in electrical transport measurements through boron-substituted GNRs suspended between the tip and the sample of a scanning tunneling microscope. First-principle simulations find that boron pairs induce a spin 1, which is modified by tuning the spacing between pairs. Our results demonstrate a route to embed spin chains in GNRs, turning them into basic elements of spintronic devices.
60 citations
TL;DR: It is shown that sublattice imbalanced nanostructures can be incorporated along a large band gap armchair graphene nanoribbon on the basis of asymmetric zigzag edge extensions, achieved by incorporating specifically designed precursor monomers.
Abstract: Exact positioning of sublattice imbalanced nanostructures in graphene nanomaterials offers a route to control interactions between induced local magnetic moments and to obtain graphene nanomaterials with magnetically nontrivial ground states. Here, we show that such sublattice imbalanced nanostructures can be incorporated along a large band gap armchair graphene nanoribbon on the basis of asymmetric zigzag edge extensions, achieved by incorporating specifically designed precursor monomers. Scanning tunneling spectroscopy of an isolated and electronically decoupled zigzag edge extension reveals Hubbard-split states in accordance with theoretical predictions. Mean-field Hubbard-based modeling of pairs of such zigzag edge extensions reveals ferromagnetic, antiferromagnetic, or quenching of the magnetic interactions depending on the relative alignment of the asymmetric edge extensions. Moreover, a ferromagnetic spin chain is demonstrated for a periodic pattern of zigzag edge extensions along the nanoribbon axis. This work opens a route toward the fabrication of graphene nanoribbon-based spin chains with complex magnetic ground states.
56 citations
TL;DR: The on-surface synthesis of atomically precise nanographenes and their atomic-scale characterization on a gold substrate by using low-temperature noncontact atomic force microscopy and scanning tunneling spectroscopy clearly reveals the emergence of magnetism in nanographenees and provides an efficient way to further explore the carbon-based magnetism.
Abstract: Nanographenes with sublattice imbalance host a net spin according to Lieb's theorem for bipartite lattices. Here, we report the on-surface synthesis of atomically precise nanographenes and their atomic-scale characterization on a gold substrate by using low-temperature noncontact atomic force microscopy and scanning tunneling spectroscopy. Our results clearly confirm individual nanographenes host a single spin of S=1/2 via the Kondo effect. In covalently linked nanographene dimers, two spins are antiferromagnetically coupled with each other as revealed by inelastic spin-flip excitation spectroscopy. The magnetic exchange interaction in dimers can be well engineered by tuning the local spin density distribution near the connection region, consistent with mean-field Hubbard model calculations. Our work clearly reveals the emergence of magnetism in nanographenes and provides an efficient way to further explore the carbon-based magnetism.
51 citations
TL;DR: The first bottom‐up synthesis of NBN‐doped zigzag‐edged GNRs through surface‐assisted polymerization and cyclodehydrogenation based on two U‐shaped molecular precursors with an NBN unit preinstalled at the zIGzag edge is reported.
Abstract: We report the first bottom-up synthesis of NBN-doped zigzag-edged GNRs (NBN-ZGNR1 and NBN-ZGNR2) through surface-assisted polymerization and cyclodehydrogenation based on two U-shaped molecular precursors with an NBN unit preinstalled at the zigzag edge. The resultant zigzag-edge topologies of GNRs are elucidated by high-resolution scanning tunneling microscopy (STM) in combination with noncontact atomic force microscopy (nc-AFM). Scanning tunneling spectroscopy (STS) measurements and density functional theory (DFT) calculations reveal that the electronic structures of NBN-ZGNR1 and NBN-ZGNR2 are significantly different from those of their corresponding pristine fully-carbon-based ZGNRs. Additionally, DFT calculations predict that the electronic structures of NBN-ZGNRs can be further tailored to be gapless and metallic through one-electron oxidation of each NBN unit into the corresponding radical cations. This work reported herein provides a feasible strategy for the synthesis of GNRs with stable zigzag edges yet tunable electronic properties.
TL;DR: In this paper, an in situ doping of oxygen atoms in monolayer molybdenum disulfide (MoS2 ) is reported during the chemical vapor deposition process.
Abstract: In 2D semiconductors, doping offers an effective approach to modulate their optical and electronic properties. Here, an in situ doping of oxygen atoms in monolayer molybdenum disulfide (MoS2 ) is reported during the chemical vapor deposition process. Oxygen concentrations up to 20-25% can be reliable achieved in these doped monolayers, MoS2-x Ox . These oxygen dopants are in a form of substitution of sulfur atoms in the MoS2 lattice and can reduce the bandgap of intrinsic MoS2 without introducing in-gap states as confirmed by photoluminescence spectroscopy and scanning tunneling spectroscopy. Field effect transistors made of monolayer MoS2-x Ox show enhanced electrical performances, such as high field-effect mobility (≈100 cm2 V-1 s-1 ) and inverter gain, ultrahigh devices' on/off ratio (>109 ) and small subthreshold swing value (≈80 mV dec-1 ). This in situ oxygen doping technique holds great promise on developing advanced electronics based on 2D semiconductors.
TL;DR: Gate-tuned scanning tunneling spectroscopy is used to directly demonstrate the tunability of the band structure of TDBG with an electric field and to show spectroscopic signatures of electronic correlations and topology for its flat band.
Abstract: Moir\'e superlattices created by the twisted stacking of two-dimensional crystalline monolayers can host electronic bands with flat energy dispersion in which interaction among electrons is strongly enhanced. These superlattices can also create non-trivial electronic band topologies making them a platform for study of many-body topological quantum states. Among the moir\'e systems realized to date, there are those predicted to have band structures and properties which can be controlled with a perpendicular electric field. The twisted double bilayer graphene (TDBG), where two Bernal bilayer graphene are stacked with a twist angle, is such a tunable moir\'e system, for which partial filling of its flat band, transport studies have found correlated insulating states. Here we use gate-tuned scanning tunneling spectroscopy (GT-STS) to directly demonstrate the tunability of the band structure of TDBG with an electric field and to show spectroscopic signatures of both electronic correlations and topology for its flat band. Our spectroscopic experiments show excellent agreement with a continuum model of TDBG band structure and reveal signatures of a correlated insulator gap at partial filling of its isolated flat band. The topological properties of this flat band are probed with the application of a magnetic field, which leads to valley polarization and the splitting of Chern bands that respond strongly to the field with a large effective g-factor. Our experiments advance our understanding of the properties of TDBG and set the stage for further investigations of correlation and topology in such tunable moir\'e systems.
TL;DR: In this article, the authors studied the local electronic properties of a NbN film with scanning tunneling spectroscopy (STS) and showed that the inhomogeneous spatial distribution of Δ is locally strongly correlated to a large depletion in the local density of states (LDOS) around the Fermi level, associated to the Altshuler-Aronov effect induced by strong electronic interactions.
Abstract: Disorder has different profound effects on superconducting thin films. For a large variety of materials, increasing disorder reduces electronic screening which enhances electron-electron repulsion. These fermionic effects lead to a mechanism described by Finkelstein: when disorder combined to electron-electron interactions increases, there is a global decrease of the superconducting energy gap Δ and of the critical temperature T$_{c}$, the ratio Δ/kBT$_{c}$ remaining roughly constant. In addition, in most films an emergent granularity develops with increasing disorder and results in the formation of inhomogeneous superconducting puddles. These gap inhomogeneities are usually accompanied by the development of bosonic features: a pseudogap develops above the critical temperature T$_{c}$ and the energy gap Δ starts decoupling from T$_{c}$. Thus the mechanism(s) driving the appearance of these gap inhomogeneities could result from a complicated interplay between fermionic and bosonic effects. By studying the local electronic properties of a NbN film with scanning tunneling spectroscopy (STS) we show that the inhomogeneous spatial distribution of Δ is locally strongly correlated to a large depletion in the local density of states (LDOS) around the Fermi level, associated to the Altshuler-Aronov effect induced by strong electronic interactions. By modelling quantitatively the measured LDOS suppression, we show that the latter can be interpreted as local variations of the film resistivity. This local change in resistivity leads to a local variation of Δ through a local Finkelstein mechanism. Our analysis furnishes a purely fermionic scenario explaining quantitatively the emergent superconducting inhomogeneities, while the precise origin of the latter remained unclear up to now.
TL;DR: The on‐surface synthesis and a proof‐of‐principle experimental study of magnetism in covalently bonded triangulene dimers are presented and collective singlet–triplet spin excitations in the dimers revealed, demonstrating efficient intertriangulenes magnetic coupling.
Abstract: Triangular zigzag nanographenes, such as triangulene and its π-extended homologues, have received widespread attention as organic nanomagnets for molecular spintronics, and may serve as building blocks for high-spin networks with long-range magnetic order, which are of immense fundamental and technological relevance. As a first step towards these lines, we present the on-surface synthesis and a proof-of-principle experimental study of magnetism in covalently bonded triangulene dimers. On-surface reactions of rationally designed precursor molecules on Au(111) lead to the selective formation of triangulene dimers in which the triangulene units are either directly connected through their minority sublattice atoms, or are separated via a 1,4-phenylene spacer. The chemical structures of the dimers have been characterized by bond-resolved scanning tunneling microscopy. Scanning tunneling spectroscopy and inelastic electron tunneling spectroscopy measurements reveal collective singlet-triplet spin excitations in the dimers, demonstrating efficient intertriangulene magnetic coupling.
TL;DR: A protocol is explored to disentangle topologically non-trivial Majorana bound states by artificially augmenting a candidate Majorana spin chain with orbitally-compatible nonmagnetic atoms, and the realization of designer Majorana chain networks for demonstrating topological quantum computation.
Abstract: Chains of magnetic atoms with either strong spin-orbit coupling or spiral magnetic order which are proximity-coupled to superconducting substrates can host topologically non-trivial Majorana bound states. The experimental signature of these states consists of spectral weight at the Fermi energy which is spatially localized near the ends of the chain. However, topologically trivial Yu-Shiba-Rusinov in-gap states localized near the ends of the chain can lead to similar spectra. Here, we explore a protocol to disentangle these contributions by artificially augmenting a candidate Majorana spin chain with orbitally-compatible nonmagnetic atoms. Combining scanning tunneling spectroscopy with ab-initio and tight-binding calculations, we realize a sharp spatial transition between the proximity-coupled spiral magnetic order and the non-magnetic superconducting wire termination, with persistent zero-energy spectral weight localized at either end of the magnetic spiral. Our findings open a new path towards the control of the spatial position of in-gap end states, trivial or Majorana, via different chain terminations, and the realization of designer Majorana chain networks for demonstrating topological quantum computation.
TL;DR: In this paper, the authors show that ultraviolet light (wavelength = 365 nm) exposure induces an extremely long-living giant photoconductivity (GPPC) in monolayer MoS2 (ML-MoS2) field effect transistors (FETs) with a time constant of ~30 days.
Abstract: Monolayer transition metal dichalcogenides (TMD) have numerous potential applications in ultrathin electronics and photonics. The exposure of TMD based devices to light generates photo-carriers resulting in an enhanced conductivity, which can be effectively used, e.g., in photodetectors. If the photo-enhanced conductivity persists after removal of the irradiation, the effect is known as persistent photoconductivity (PPC). Here we show that ultraviolet light (wavelength = 365 nm) exposure induces an extremely long-living giant PPC (GPPC) in monolayer MoS2 (ML-MoS2) field-effect transistors (FET) with a time constant of ~30 days. Furthermore, this effect leads to a large enhancement of the conductivity up to a factor of 107. In contrast to previous studies in which the origin of the PPC was attributed to extrinsic reasons such as trapped charges in the substrate or adsorbates, we unambiguously show that the GPPC arises mainly from the intrinsic properties of ML-MoS2 such as lattice defects that induce a large amount of localized states in the forbidden gap. This finding is supported by a detailed experimental and theoretical study of the electric transport in TMD based FETs as well as by characterization of ML-MoS2 with scanning tunneling spectroscopy, high-resolution transmission electron microscopy, and photoluminescence measurements. The obtained results provide a basis towards the defect-based engineering of the electronic and optical properties of TMDs for device applications.
TL;DR: A new strategy to visualize single metallo-polymer chain with hexameric or trimeric supramolecule as repeat unit is demonstrated, in which Ru(II) with strong coordination and Fe( II) with weak coordination were combined together in a step-wise manner.
Abstract: During the past few decades, the study of the single polymer chain has attracted considerable attention with the goal of exploring the structure-property relationship of polymers. It still, however, remains challenging due to the variability and low atomic resolution of the amorphous single polymer chain. Here, we demonstrated a new strategy to visualize the single metallopolymer chain with a hexameric or trimeric supramolecule as a repeat unit, in which Ru(II) with strong coordination and Fe(II) with weak coordination were combined together in a stepwise manner. With the help of ultrahigh-vacuum, low-temperature scanning tunneling microscopy (UHV-LT-STM) and scanning tunneling spectroscopy (STS), we were able to directly visualize both Ru(II) and Fe(II), which act as staining reagents on the repeat units, thus providing detailed structural information for the single polymer chain. As such, the direct visualization of the single random polymer chain is realized to enhance the characterization of polymers at the single-molecule level.
TL;DR: In this paper, the authors used scanning tunneling spectroscopy to image spinon density modulations arising from a spinon Fermi surface instability in single-layer 1T-TaSe$_2$, a two-dimensional Mott insulator.
Abstract: Two-dimensional triangular-lattice antiferromagnets are predicted under some conditions to exhibit a quantum spin liquid ground state whose low-energy behavior is described by a spinon Fermi surface. Directly imaging the resulting spinons, however, is difficult due to their fractional, chargeless nature. Here we use scanning tunneling spectroscopy to image spinon density modulations arising from a spinon Fermi surface instability in single-layer 1T-TaSe$_2$, a two-dimensional Mott insulator. We first demonstrate the existence of localized spins arranged on a triangular lattice in single-layer 1T-TaSe$_2$ by contacting it to a metallic 1H-TaSe$_2$ layer and measuring the Kondo effect. Subsequent spectroscopic imaging of isolated, single-layer 1T-TaSe$_2$ reveals long-wavelength modulations at Hubbard band energies that reflect spinon density modulations. This allows direct experimental measurement of the spinon Fermi wavevector, in good agreement with theoretical predictions for a 2D quantum spin liquid. These results establish single-layer 1T-TaSe$_2$ as a new platform for studying novel two-dimensional quantum-spin-liquid phenomena.
TL;DR: In this article, the authors analyzed the interdependence of Kondo screening and superconductivity and showed that the coupling and the resulting YSR states are strongly adsorption site-dependent and reveal a quantum phase transition at a Kondo temperature comparable to the superconducting gap.
Abstract: The coupling of a spin to an underlying substrate is the basis for a plethora of phenomena In the case of a metallic substrate, Kondo screening of the adatom magnetic moment can occur As the substrate turns superconducting, an intriguing situation emerges where pair breaking due to the adatom spins leads to Yu-Shiba-Rusinov bound states, but also intertwines with Kondo phenomena Through scanning tunneling spectroscopy, we analyze the interdependence of Kondo screening and superconductivity Our data obtained on single Fe adatoms on Nb(110) show that the coupling and the resulting YSR states are strongly adsorption site-dependent and reveal a quantum phase transition at a Kondo temperature comparable to the superconducting gap The experimental signatures are rationalized by combined density-functional theory and continuous-time quantum Monte Carlo calculations to rigorously treat magnetic and hybridization effects on equal footing
TL;DR: It is shown that the plane-contacted perovskite and graphene interface presents a lower barrier than gold for charge injection, and layer-dependent tunneling barrier and domain size on few-layered Ruddlesden-Popper perovkite is revealed.
Abstract: Quasi-two-dimensional perovskites have emerged as a new material platform for optoelectronics on account of its intrinsic stability. A major bottleneck to device performance is the high charge injection barrier caused by organic molecular layers on its basal plane, thus the best performing device currently relies on edge contact. Herein, by leveraging on van der Waals coupling and energy level matching between two-dimensional Ruddlesden-Popper perovskite and graphene, we show that the plane-contacted perovskite and graphene interface presents a lower barrier than gold for charge injection. Electron tunneling across the interface occurs via a gate-tunable, direct tunneling-to-field emission mechanism with increasing bias, and photoinduced charge transfer occurs at femtosecond timescale (~50 fs). Field effect transistors fabricated on molecularly thin Ruddlesden-Popper perovskite using graphene contact exhibit electron mobilities ranging from 0.1 to 0.018 cm2V−1s−1 between 1.7 to 200 K. Scanning tunneling spectroscopy studies reveal layer-dependent tunneling barrier and domain size on few-layered Ruddlesden-Popper perovskite. Insulating molecular layers on the basal plane of 2D perovskite is a major bottleneck for charge injection that limiting device performance. Here, the authors show that plane-contacted graphene functions as a low barrier and gate-tunable contact to overcome this limitation.
TL;DR: The design and on-surface synthesis of NGs containing several odd-membered polycycles induced by a thermal procedure on Au(111) are reported and surface-catalyzed skeletal ring rearrangement reactions in the NGs lead to the formation of additional hep-tagonal rings as well as pentalene and as-indacene units in 2A and 2B, respectively.
Abstract: Nanographenes (NGs) have gained increasing attention due to their immense potential as tailor-made organic materials for nanoelectronics and spintronics. They exhibit a rich spectrum of physicochemical properties that can be tuned by controlling the size or the edge structure or by introducing structural defects in the honeycomb lattice. Here, we report the design and on-surface synthesis of NGs containing several odd-membered polycycles induced by a thermal procedure on Au(111). Our scanning tunneling microscopy, noncontact atomic force microscopy, and scanning tunneling spectroscopy measurements, complemented by computational investigations, describe the formation of two nonbenzenoid NGs (2A,B) containing four embedded azulene units in the polycyclic framework, via on-surface oxidative ring-closure reactions. Interestingly, we observe surface-catalyzed skeletal ring rearrangement reactions in the NGs, which lead to the formation of additional heptagonal rings as well as pentalene and as-indacene units in 2A,B, respectively. 2A,B on Au(111) both exhibit narrow experimental frontier electronic gaps of 0.96 and 0.85 eV, respectively, and Fermi level pinning of their HOMOs together with considerable electron transfer to the substrate. Ab initio calculations estimate moderate open-shell biradical characters for the NGs in the gas phase.
TL;DR: The results establish a bias-dependent STM signature of the Bi2Te3native defects and shed light on the link between the native defects and the electronic properties of Bi2 Te3, which is relevant for the synthesis of topological insulator materials and the related functional properties.
Abstract: We successfully identified native point defects that occur in Bi2Te3 crystals by combining high-resolution bias-dependent scanning tunneling microscopy and density functional theory based calculations. As-grown Bi2Te3 crystals contain vacancies, antisites, and interstitial defects that may result in bulk conductivity and therefore may change the insulating bulk character. Here, we demonstrate the interplay between the growth conditions and the density of different types of native near-surface defects. In particular, scanning tunneling spectroscopy reveals the dependence on not only the local atomic environment but also on the growth kinetics and the resulting sample doping from n-type toward intrinsic crystals with the Fermi level positioned inside the energy gap. Our results establish a bias-dependent STM signature of the Bi2Te3 native defects and shed light on the link between the native defects and the electronic properties of Bi2Te3, which is relevant for the synthesis of topological insulator materials and the related functional properties.
TL;DR: This work grows high-quality armchair graphene nanoribbons on the sidewalls of 6H-SiC mesa structures and demonstrates an ideal one-dimensional electronic behavior that is realized in a graphene-based environment, consisting of well-resolved subbands, dispersing and non-dispersing along and across the ribbons respectively.
Abstract: The ability to define an off state in logic electronics is the key ingredient that is impossible to fulfill using a conventional pristine graphene layer, due to the absence of an electronic bandgap. For years, this property has been the missing element for incorporating graphene into next-generation field effect transistors. In this work, we grow high-quality armchair graphene nanoribbons on the sidewalls of 6H-SiC mesa structures. Angle-resolved photoelectron spectroscopy (ARPES) and scanning tunneling spectroscopy measurements reveal the development of a width-dependent semiconducting gap driven by quantum confinement effects. Furthermore, ARPES demonstrates an ideal one-dimensional electronic behavior that is realized in a graphene-based environment, consisting of well-resolved subbands, dispersing and non-dispersing along and across the ribbons respectively. Our experimental findings, coupled with theoretical tight-binding calculations, set the grounds for a deeper exploration of quantum confinement phenomena and may open intriguing avenues for new low-power electronics.
TL;DR: A joint experimental and theoretical study of the electronic structure of boroxine-linked COFs grown under ultra-high vacuum conditions and characterized using scanning tunneling spectroscopy on Au(111) and hBN/Cu(111), showing that a single hBN layer electronically decouples the COF from the metallic substrate.
Abstract: Covalent organic frameworks (COFs) are molecule-based 2D and 3D materials that possess a wide range of mechanical and electronic properties. We have performed a joint experimental and theoretical study of the electronic structure of boroxine-linked COFs grown under ultrahigh vacuum conditions and characterized using scanning tunneling spectroscopy on Au(111) and hBN/Cu(111) substrates. Our results show that a single hBN layer electronically decouples the COF from the metallic substrate, thus suppressing substrate-induced broadening and revealing new features in the COF electronic local density of states (LDOS). The resulting sharpening of LDOS features allows us to experimentally determine the COF band gap, bandwidths, and the electronic hopping amplitude between adjacent COF bridge sites. These experimental parameters are consistent with the results of first-principles theoretical predictions.
TL;DR: An atomic-scale MIT triggered by surface termination conversion in SrRuO3 ultrathin films is reported, introducing a new paradigm to stimulate and tune exotic functionalities of oxide heterostructures with atomic precision.
Abstract: The metal-insulator transition (MIT) in transition-metal-oxide is fertile ground for exploring intriguing physics and potential device applications. Here, an atomic-scale MIT triggered by surface termination conversion in SrRuO3 ultrathin films is reported. Uniform and effective termination engineering at the SrRuO3 (001) surface can be realized via a self-limiting water-leaching process. As the surface termination converts from SrO to RuO2 , a highly insulating and nonferromagnetic phase emerges within the topmost SrRuO3 monolayer. Such a spatially confined MIT is corroborated by systematic characterizations on electrical transport, magnetism, and scanning tunneling spectroscopy. Density functional theory calculations and X-ray linear dichroism further suggest that the surface termination conversion breaks the local octahedral symmetry of the crystal field. The resultant modulation in 4d orbital occupancy stabilizes a nonferromagnetic insulating surface state. This work introduces a new paradigm to stimulate and tune exotic functionalities of oxide heterostructures with atomic precision.
TL;DR: It is shown that both asymmetries originate in interfering tunneling paths via a spin-carrying orbital and the highest occupied molecular orbital (HOMO) and are established an important mechanism for the asymmetry of Kondo and YSR line shapes.
Abstract: Magnetic adsorbates on superconductors induce a Kondo resonance outside and Yu-Shiba-Rusinov (YSR) bound states inside the superconducting energy gap. When probed by scanning tunneling spectroscopy, the associated differential-conductance spectra frequently exhibit characteristic bias-voltage asymmetries. Here, we observe correlated variations of Kondo and YSR asymmetries across an Fe-porphyrin molecule adsorbed on Pb(111). We show that both asymmetries originate in interfering tunneling paths via a spin-carrying orbital and the highest occupied molecular orbital (HOMO). Strong evidence for this model comes from nodal planes of the HOMO, where tunneling reveals symmetric Kondo and YSR resonances. Our results establish an important mechanism for the asymmetries of Kondo and YSR line shapes.
TL;DR: D density functional theory calculations elucidate the origin of band bending and charging at these 1D defects in Mo2 and show that the line charge can also be assessed from the filling of the boundary-localized electronic band and the charge induced by the polarization discontinuity across the defect.
Abstract: The variation of the electronic structure normal to 1D defects in quasi-freestanding MoS2, grown by molecular beam epitaxy, is investigated through high resolution scanning tunneling spectroscopy a...
TL;DR: In this paper, in situ scanning tunneling spectroscopy was used to detect the ZEBSs upon the interstitial Fe adatoms deposited on two different high-temperature superconducting one-unit-cell iron chalcogenides on SrTiO3(001).
Abstract: Majorana zero modes (MZMs) that obey the non-Abelian statistics have been intensively investigated for potential applications in topological quantum computing. The prevailing signals in tunneling experiments "fingerprinting" the existence of MZMs are the zero-energy bound states (ZEBSs). However, nearly all of the previously reported ZEBSs showing signatures of the MZMs are observed in difficult-to-fabricate heterostructures at very low temperatures and additionally require applied magnetic field. Here, by using in situ scanning tunneling spectroscopy, we detect the ZEBSs upon the interstitial Fe adatoms deposited on two different high-temperature superconducting one-unit-cell iron chalcogenides on SrTiO3(001). The spectroscopic results resemble the phenomenological characteristics of the MZMs inside the vortex cores of topological superconductors. Our experimental findings may extend the MZM explorations in connate topological superconductors toward an applicable temperature regime and down to the two-dimensional (2D) limit.
TL;DR: The stability of the antiferroelastic structure drives the collective spin-state switching of multiple Ni atoms in the same chain in response to electron/hole tunneling to a Ni atom via a domino-like magneto-structural relaxation process.
Abstract: Coupled spin-crossover complexes in supramolecular systems feature rich spin phases that can exhibit collective behaviors. Here, we report on a molecular-level exploration of the spin phase and col...