Wenzhi Lin

Electronic Bandgap and Edge Reconstruction in Phosphorene Materials

Single-layer black phosphorus (BP), or phosphorene, is a highly anisotropic two-dimensional elemental material possessing promising semiconductor properties for flexible electronics. However, the direct bandgap of single-layer black phosphorus predicted theoretically has not been directly measured, and the properties of its edges have not been considered in detail. Here we report atomic scale electronic variation related to strain-induced anisotropic deformation of the puckered honeycomb structure of freshly cleaved black phosphorus using a high-resolution scanning tunneling spectroscopy (STS) survey along the light (x) and heavy (y) effective mass directions. Through a combination of STS measurements and first-principles calculations, a model for edge reconstruction is also determined. The reconstruction is shown to self-passivate most dangling bonds by switching the coordination number of phosphorus from 3 to 5 or 3 to 4.

Atomically resolved spectroscopic study of Sr2IrO4: Experiment and theory

Particularly in Sr2IrO4, the interplay between spin-orbit coupling, bandwidth and on-site Coulomb repulsion stabilizes a Jeff = 1/2 spin-orbital entangled insulating state at low temperatures. Whether this insulating phase is Mott- or Slater-type, has been under intense debate. We address this issue via spatially resolved imaging and spectroscopic studies of the Sr2IrO4 surface using scanning tunneling microscopy/spectroscopy (STM/S). STS results clearly illustrate the opening of an insulating gap (150 ~ 250 meV) below the Néel temperature (TN), in qualitative agreement with our density-functional theory (DFT) calculations. More importantly, the temperature dependence of the gap is qualitatively consistent with our DFT + dynamical mean field theory (DMFT) results, both showing a continuous transition from a gapped insulating ground state to a non-gap phase as temperatures approach TN. These results indicate a significant Slater character of gap formation, thus suggesting that Sr2IrO4 is a uniquely correlated system, where Slater and Mott-Hubbard-type behaviors coexist.

Direct Probe of Interplay between Local Structure and Superconductivity in FeTe0.55Se0.45

The relationship between atomically defined structures and physical properties in functional materials remains a subject of constant interest. We explore the interplay between local crystallographic structure, composition, and local superconductive properties in iron chalcogenide superconductors. Direct structural analysis of scanning tunneling microscopy data allows local lattice distortions and structural defects across an FeTe0.55Se0.45 surface to be explored on a single unit-cell level. Concurrent superconducting gap (SG) mapping reveals suppression of the SG at well-defined structural defects, identified as a local structural distortion. The strong structural distortion causes the vanishing of the superconducting state. This study provides insight into the origins of superconductivity in iron chalcogenides by providing an example of atomic-level studies of the structure-property relationship.

Research Update: Spatially resolved mapping of electronic structure on atomic level by multivariate statistical analysis

Atomic level spatial variability of electronic structure in Fe-based superconductor FeTe0.55Se0.45 (Tc = 15 K) is explored using current-imaging tunneling-spectroscopy. Multivariate statistical analysis of the data differentiates regions of dissimilar electronic behavior that can be identified with the segregation of chalcogen atoms, as well as boundaries between terminations and near neighbor interactions. Subsequent clustering analysis allows identification of the spatial localization of these dissimilar regions. Similar statistical analysis of modeled calculated density of states of chemically inhomogeneous FeTe1−xSex structures further confirms that the two types of chalcogens, i.e., Te and Se, can be identified by their electronic signature and differentiated by their local chemical environment. This approach allows detailed chemical discrimination of the scanning tunneling microscopy data including separation of atomic identities, proximity, and local configuration effects and can be universally app...

Chemically induced Jahn–Teller ordering on manganite surfaces

Physical and electrochemical phenomena at the surfaces of transition metal oxides and their coupling to local functionality remains one of the enigmas of condensed matter physics. Understanding the emergent physical phenomena at surfaces requires the capability to probe the local composition, map order parameter fields and establish their coupling to electronic properties. Here we demonstrate that measuring the sub-30-pm displacements of atoms from high-symmetry positions in the atomically resolved scanning tunnelling microscopy allows the physical order parameter fields to be visualized in real space on the single-atom level. Here, this local crystallographic analysis is applied to the in-situ-grown manganite surfaces. In particular, using direct bond-angle mapping we report direct observation of structural domains on manganite surfaces, and trace their origin to surface-chemistry-induced stabilization of ordered Jahn-Teller displacements. Density functional calculations provide insight into the intriguing interplay between the various degrees of freedom now resolved on the atomic level.

Modification of the electronic properties of hexagonal boron-nitride in BN/graphene vertical heterostructures

Van der Waals (vdW) heterostructures consist of isolated atomic planar structures, assembled layer-by-layer into desired structures in a well-defined sequence. Graphene deposited on hexagonal boron nitride (h-BN) has been first considered as a testbed system for vdW heterostructures, and many others have been demonstrated both theoretically and experimentally, revealing many attractive properties and phenomena. However, much less emphasis has been placed on how graphene actively affects h-BN properties. Here, we perform local probe measurements on single-layer h-BN grown over graphene and highlight the manifestation of a proximity effect that significantly affects the electronic properties of h-BN due to its coupling with the underlying graphene. We find electronic states originating from the graphene layer and the Cu substrate to be injected into the wide electronic gap of the h-BN top layer. Such proximity effect is further confirmed in a study of the variation of h-BN in-gap states with interlayer couplings, elucidated using a combination of topographical/spectroscopic measurements and first-principles density functional theory calculations. The findings of this work indicate the potential of mutually engineering electronic properties of the components of vdW heterostructures.

Local crystallography analysis for atomically resolved scanning tunneling microscopy images

Scanning probe microscopy has emerged as a powerful and flexible tool for atomically resolved imaging of surface structures. However, due to the amount of information extracted, in many cases the interpretation of such data is limited to being qualitative and semi-quantitative in nature. At the same time, much can be learned from local atom parameters, such as distances and angles, that can be analyzed and interpreted as variations of local chemical bonding, or order parameter fields. Here, we demonstrate an iterative algorithm for indexing and determining atomic positions that allows the analysis of inhomogeneous surfaces. This approach is further illustrated by local crystallographic analysis of several real surfaces, including highly ordered pyrolytic graphite and an Fe-based superconductor FeTe0.55Se0.45. This study provides a new pathway to extract and quantify local properties for scanning probe microscopy images.

Temperature-composition phase diagrams for Ba1−xSrxFe2As2(0≤x≤1) and superconducting Ba0.5Sr0.5(Fe1−yCoy)2As2(0≤y≤0.141)

Single crystals of mixed alkaline earth metal iron arsenide materials of Ba1-xSrxFe2As2 and Ba0.5Sr0.5(Fe1-yCoy)2As2 are synthesized via the self-flux method. Ba1-xSrxFe2As2 display spin-density wave features (TN) at temperatures intermediate to the parent materials, x = 0 and 1, with TN(x) following an approximately linear trend. Cobalt doping of the 1 to 1 Ba:Sr mixture, Ba0.5Sr0.5(Fe1-yCoy)2As2, results in a superconducting dome with maximum transition temperature of TC = 19 K at y = 0.092, close to the maximum transition temperatures observed in unmixed A(Fe1-yCoy)2As2; however, an annealed crystal with y = 0.141 showed a TC increase from 11 to 16 K with a decrease in Sommerfeld coefficient from 2.58(2) to 0.63(2) mJ/(K2 mol atom). For the underdoped y = 0.053, neutron diffraction results give evidence that TN and structural transition (To) are linked at 78 K, with anomalies observed in magnetization, resistivity and heat capacity data, while a superconducting transition at TC ~ 6 K is seen in resistivity and heat capacity data. Scanning tunneling microscopy measurements for y = 0.073 give Dynes broadening factor of 1.15 and a superconducting gap of 2.37 meV with evidence of surface inhomogeneity.

On the role of chalcogen vapor annealing in inducing bulk superconductivity in Fe

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