Atomic-scale probing of heterointerface phonon bridges in nitride semiconductor.

Interface phonon modes that are generated by several atomic layers at the heterointerface play a major role in the interface thermal conductance for nanoscale high-power devices such as nitride-based high-electron-mobility transistors and light-emitting diodes. Here we measure the local phonon spectra across AlN/Si and AlN/Al interfaces using atomically resolved vibrational electron energy-loss spectroscopy in a scanning transmission electron microscope. At the AlN/Si interface, we observe various interface phonon modes, of which the extended and localized modes act as bridges to connect the bulk AlN modes and bulk Si modes and are expected to boost the phonon transport, thus substantially contributing to interface thermal conductance. In comparison, no such phonon bridge is observed at the AlN/Al interface, for which partially extended modes dominate the interface thermal conductivity. This work provides valuable insights into understanding the interfacial thermal transport in nitride semiconductors and useful guidance for thermal management via interface engineering.

Chiral Charge Density Wave and Backscattering-Immune Orbital Texture in Monolayer 1T-TiTe2.

Nontrivial electronic states are attracting intense attention in low-dimensional physics. Though chirality has been identified in charge states with a scalar order parameter, its intertwining with charge density waves (CDW), film thickness, and the impact on the electronic behaviors remain less well understood. Here, using scanning tunneling microscopy, we report a 2 × 2 chiral CDW as well as a strong suppression of the Te-5p hole-band backscattering in monolayer 1T-TiTe2. These exotic characters vanish in bilayer TiTe2 in a non-CDW state. Theoretical calculations prove that chirality comes from a helical stacking of the triple-q CDW components and, therefore, can persist at the two-dimensional limit. Furthermore, the chirality renders the Te-5p bands with an unconventional orbital texture that prohibits electron backscattering. Our study establishes TiTe2 as a promising playground for manipulating the chiral ground states at the monolayer limit and provides a novel path to engineer electronic properties from an orbital degree.

Semiconductor-Metal Phase Transition and Emergent Charge Density Waves in 1T-ZrX2 (X = Se, Te) at the Two-Dimensional Limit.

A charge density wave (CDW) is a collective quantum phenomenon in metals and features a wavelike modulation of the conduction electron density. A microscopic understanding and experimental control of this many-body electronic state in atomically thin materials remain hot topics in materials physics. By means of material engineering, we realized a dimensionality and Zr intercalation induced semiconductor-metal phase transition in 1T-ZrX2 (X = Se, Te) ultrathin films, accompanied by a commensurate 2 × 2 CDW order. Furthermore, we observed a CDW energy gap of up to 22 meV around the Fermi level. Fourier-transformed scanning tunneling microscopy and angle-resolved photoemission spectroscopy reveal that 1T-ZrX2 films exhibit the simplest Fermi surface among the known CDW materials in TMDCs, consisting only of a Zr 4d derived elliptical electron conduction band at the corners of the Brillouin zone.

Direct Observation of Full-Gap Superconductivity and Pseudogap in Two-Dimensional Fullerides.

Alkali-fulleride superconductors with a maximum critical temperature T_{c}∼40 K exhibit a similar electronic phase diagram to that of unconventional high-T_{c} superconductors. Here we employ cryogenic scanning tunneling microscopy to show that trilayer K_{3}C_{60} displays fully gapped strong coupling s-wave superconductivity, accompanied by a pseudogap above T_{c}∼22 K and within vortices. A precise control of the electronic correlations and potassium doping enables us to reveal that superconductivity occurs near a superconductor-Mott-insulator transition and reaches maximum at half-filling. The s-wave symmetry retains over the entire phase diagram, which, in conjunction with an abrupt decline of the superconductivity below half-filling, indicates that alkali fullerides are predominantly phonon-mediated superconductors, although the electronic correlations also come into play.

Direct Visualization of Ambipolar Mott Transition in Cuprate CuO_{2} Planes.

Identifying the essence of doped Mott insulators is one of the major outstanding problems in condensed matter physics and the key to understanding the high-temperature superconductivity in cuprates. We report real space visualization of Mott insulator-metal transition in Sr_{1-x}La_{x}CuO_{2+y} cuprate films that cover both the electron- and hole-doped regimes. Tunneling conductance measurements directly on the copper-oxide (CuO_{2}) planes reveal a systematic shift in the Fermi level, while the fundamental Mott-Hubbard band structure remains unchanged. This is further demonstrated by exploring the atomic-scale electronic response of CuO_{2} to substitutional dopants and intrinsic defects in a sister compound Sr_{0.92}Nd_{0.08}CuO_{2}. The results may be better explained in the framework of self-modulation doping, similar to that in semiconductor heterostructures, and form a basis for developing any microscopic theories for cuprate superconductivity.

Edge States at Nematic Domain Walls in FeSe Films.

Quantum spin Hall (QSH) effect is an intriguing phenomenon arising from the helical edge states in two-dimensional topological insulators. We use molecular beam epitaxy (MBE) to prepare FeSe films with atomically sharp nematic domain boundaries, where tensile strains, nematicity suppression, and topological band inversion are simultaneously achieved. Using scanning tunneling microscopy (STM), we observe edge states at the Fermi level that spatially distribute as two distinct strips in the vicinity of the domain boundaries. At the end point of the boundaries, a bound state at the Fermi level is further observed. The topological origin of the edge states is supported by density functional theory calculations. Our findings not only demonstrate a candidate for QSH states but also provide a new pathway to realize topological superconductivity in a single-component film.

Topological edge states in a high-temperature superconductor FeSe/SrTiO3(001) film.

Superconducting and topological states are two most intriguing quantum phenomena in solid materials. The entanglement of these two states, the topological superconducting state, will give rise to even more exotic quantum phenomena. While many materials are found to be either a superconductor or a topological insulator, it is very rare that both states exist in one material. Here, we demonstrate by first-principles theory as well as scanning tunnelling spectroscopy and angle-resolved photoemission spectroscopy experiments that the recently discovered 'two-dimensional (2D) superconductor' of single-layer FeSe also exhibits 1D topological edge states within an energy gap of ∼40 meV at the M point below the Fermi level. It is the first 2D material that supports both superconducting and topological states, offering an exciting opportunity to study 2D topological superconductors through the proximity effect.

Dumbbell Defects in FeSe Films: A Scanning Tunneling Microscopy and First-Principles Investigation.

The properties of iron-based superconductors (Fe-SCs) can be varied dramatically with the introduction of dopants and atomic defects. As a pressing example, FeSe, parent phase of the highest-Tc Fe-SC, exhibits prevalent defects with atomic-scale "dumbbell" signatures as imaged by scanning tunneling microscopy (STM). These defects spoil superconductivity when their concentration exceeds 2.5%. Resolving their chemical identity is a prerequisite to applications such as nanoscale patterning of superconducting/nonsuperconducting regions in FeSe as well as fundamental questions such as the mechanism of superconductivity and the path by which the defects destroy it. We use STM and density functional theory to characterize and identify the dumbbell defects. In contrast to previous speculations about Se adsorbates or substitutions, we find that an Fe-site vacancy is the most energetically favorable defect in Se-rich conditions and reproduces our observed STM signature. Our calculations shed light more generally on the nature of Se capping, the removal of Fe vacancies via annealing, and their ordering into a √5 × âˆš5 superstructure in FeSe and related alkali-doped compounds.

High-Temperature Superconductivity in Single-Unit-Cell FeSe Films on Anatase TiO_{2}(001).

We report on the observation of high-temperature (T_{c}) superconductivity and magnetic vortices in single-unit-cell FeSe films on anatase TiO_{2}(001) substrate by using scanning tunneling microscopy. A systematic study and engineering of interfacial properties has clarified the essential roles of substrate in realizing the high-T_{c} superconductivity, probably via interface-induced electron-phonon coupling enhancement and charge transfer. By visualizing and tuning the oxygen vacancies at the interface, we find their very limited effect on the superconductivity, which excludes interfacial oxygen vacancies as the primary source for charge transfer between the substrate and FeSe films. Our findings have placed severe constraints on any microscopic model for the high-T_{c} superconductivity in FeSe-related heterostructures.

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

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

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

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

Revealing the Empty-State Electronic Structure of Single-Unit-Cell FeSe/SrTiO3.

We use scanning tunneling spectroscopy to investigate the filled and empty electronic states of superconducting single-unit-cell FeSe deposited on SrTiO3(001). We map the momentum-space band structure by combining quasiparticle interference imaging with decay length spectroscopy. In addition to quantifying the filled-state bands, we discover a Γ-centered electron pocket 75 meV above the Fermi energy. Our density functional theory calculations show the orbital nature of empty states at Γ and explain how the Se height is a key tuning parameter of their energies, with broad implications for electronic properties.

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

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

Detection of a superconducting phase in a two-atom layer of hexagonal Ga film grown on semiconducting GaN(0001).

The recent observation of the superconducting state at atomic scale has motivated the pursuit of exotic condensed phases in two-dimensional (2D) systems. Here we report on a superconducting phase in two-monolayer crystalline Ga films epitaxially grown on wide-band-gap semiconductor GaN(0001). This phase exhibits a hexagonal structure and only 0.552 nm in thickness, nevertheless, brings about a superconducting transition temperature Tc as high as 5.4 K, confirmed by in situ scanning tunneling spectroscopy and ex situ electrical magnetotransport and magnetization measurements. The anisotropy of critical magnetic field and Berezinski-Kosterlitz-Thouless-like transition are observed, typical for the 2D superconductivity. Our results demonstrate a novel platform for exploring atomic-scale 2D superconductors, with great potential for understanding the interface superconductivity.

Imaging the electron-boson coupling in superconducting FeSe films using a scanning tunneling microscope.

Scanning tunneling spectroscopy has been used to reveal signatures of a bosonic mode in the local quasiparticle density of states of superconducting FeSe films. The mode appears below Tc as a "dip-hump" feature at energy Ω∼4.7kBTc beyond the superconducting gap Δ. Spectra on strained regions of the FeSe films reveal simultaneous decreases in Δ and Ω. This contrasts with all previous reports on other high-Tc superconductors, where Δ locally anticorrelates with Ω. A local strong coupling model is found to reconcile the discrepancy well, and to provide a unified picture of the electron-boson coupling in unconventional superconductors.

Quantum spin driven Yu-Shiba-Rusinov multiplets and fermion-parity-preserving phase transition in K3C60.

Magnetic impurities in superconductors are of increasing interest due to emergent Yu-Shiba-Rusinov (YSR) states and Majorana zero modes for fault-tolerant quantum computation. However, a direct relationship between the YSR multiple states and magnetic anisotropy splitting of quantum impurity spins remains poorly characterized. By using scanning tunneling microscopy, we systematically resolve individual transition-metal (Fe, Cr, and Ni) impurities induced YSR multiplets as well as their Zeeman effects in the K3C60 superconductor. The YSR multiplets show identical d orbital-like wave functions that are symmetry-mismatched to the threefold K3C60(1 1 1) host surface, breaking point-group symmetries of the spatial distribution of YSR bound states in real space. Remarkably, we identify an unprecedented fermion-parity-preserving quantum phase transition between ground states with opposite signs of the uniaxial magnetic anisotropy that can be manipulated by an external magnetic field. These findings can be readily understood in terms of anisotropy splitting of quantum impurity spins, and thus elucidate the intricate interplay between the magnetic anisotropy and YSR multiplets.

Critical nematic correlations throughout the superconducting doping range in Bi2-zPbzSr2-yLayCuO6+x.

Charge modulations have been widely observed in cuprates, suggesting their centrality for understanding the high-Tc superconductivity in these materials. However, the dimensionality of these modulations remains controversial, including whether their wavevector is unidirectional or bidirectional, and also whether they extend seamlessly from the surface of the material into the bulk. Material disorder presents severe challenges to understanding the charge modulations through bulk scattering techniques. We use a local technique, scanning tunneling microscopy, to image the static charge modulations on Bi2-zPbzSr2-yLayCuO6+x. The ratio of the phase correlation length ξCDW to the orientation correlation length ξorient points to unidirectional charge modulations. By computing new critical exponents at free surfaces including that of the pair connectivity correlation function, we show that these locally 1D charge modulations are actually a bulk effect resulting from classical 3D criticality of the random field Ising model throughout the entire superconducting doping range.

Landau quantization and the thickness limit of topological insulator thin films of Sb2Te3.

We report the experimental observation of Landau quantization of molecular beam epitaxy grown Sb{2}Te{3} thin films by a low-temperature scanning tunneling microscope. Different from all the reported systems, the Landau quantization in a Sb{2}Te{3} topological insulator is not sensitive to the intrinsic substitutional defects in the films. As a result, a nearly perfect linear energy dispersion of surface states as a 2D massless Dirac fermion system is achieved. We demonstrate that four quintuple layers are the thickness limit for a Sb{2}Te{3} thin film being a 3D topological insulator. The mechanism of the Landau-level broadening is discussed in terms of enhanced quasiparticle lifetime.

Fermi-level tuning of epitaxial Sb2Te3 thin films on graphene by regulating intrinsic defects and substrate transfer doping.

High-quality Sb2Te3 films are obtained by molecular beam epitaxy on a graphene substrate and investigated by in situ scanning tunneling microscopy and spectroscopy. Intrinsic defects responsible for the natural p-type conductivity of Sb2Te3 are identified to be the Sb vacancies and Sb(Te) antisites in agreement with first-principles calculations. By minimizing defect densities, coupled with a transfer doping by the graphene substrate, the Fermi level of Sb2Te3 thin films can be tuned over the entire range of the bulk band gap. This establishes the necessary condition to explore topological insulator behaviors near the Dirac point.

Suppression of superconductivity by twin boundaries in FeSe.

Low-temperature scanning tunneling microscopy and spectroscopy are employed to investigate twin boundaries in stoichiometric FeSe films grown by molecular beam epitaxy. Twin boundaries can be unambiguously identified by imaging the 90° change in the orientation of local electronic dimers from Fe site impurities on either side. Twin boundaries run at approximately 45° to the Fe-Fe bond directions, and noticeably suppress the superconducting gap, in contrast with the recent experimental and theoretical findings in other iron pnictides. Furthermore, vortices appear to accumulate on twin boundaries, consistent with the degraded superconductivity there. The variation in superconductivity is likely caused by the increased Se height in the vicinity of twin boundaries, providing the first local evidence for the importance of this height to the mechanism of superconductivity.