Christopher John Butler

Large single crystal growth, transport property, and spectroscopic characterizations of three-dimensional Dirac semimetal Cd3As2.

The three dimensional (3D) Dirac semimetal is a new quantum state of matter that has attracted much attention recently in physics and material science. Here, we report on the growth of large plate-like single crystals of Cd3As2 in two major orientations by a self-selecting vapor growth (SSVG) method, and the optimum growth conditions have been experimentally determined. The crystalline imperfections and electrical properties of the crystals were examined with transmission electron microscopy (TEM), scanning tunneling microscopy (STM), and transport property measurements. This SSVG method makes it possible to control the as-grown crystal compositions with excess Cd or As leading to mobilities near 5–105 cm2V−1s−1. Zn-doping can effectively reduce the carrier density to reach the maximum residual resistivity ratio (RRRρ300K/ρ5K) of 7.6. A vacuum-cleaved single crystal has been investigated using angle-resolved photoemission spectroscopy (ARPES) to reveal a single Dirac cone near the center of the surface Brillouin zone with a binding energy of approximately 200 meV.

Graphite edge controlled registration of monolayer MoS2 crystal orientation

Transition metal dichalcogenides such as the semiconductor MoS2 are a class of two-dimensional crystals. The surface morphology and quality of MoS2 grown by chemical vapor deposition are examined using atomic force and scanning tunneling microscopy techniques. By analyzing the moire patterns from several triangular MoS2 islands, we find that there exist at least five different superstructures and that the relative rotational angles between the MoS2 adlayer and graphite substrate lattices are typically less than 3°. We conclude that since MoS2 grows at graphite step-edges, it is the edge structure which controls the orientation of the islands, with those growing from zig-zag (or armchair) edges tending to orient with one lattice vector parallel (perpendicular) to the step-edge.

Mapping polarization induced surface band bending on the Rashba semiconductor BiTeI

Surfaces of semiconductors with strong spin-orbit coupling are of great interest for use in spintronic devices exploiting the Rashba effect. BiTeI features large Rashba-type spin splitting in both valence and conduction bands. Either can be shifted towards the Fermi level by surface band bending induced by the two possible polar terminations, making Rashba spin-split electron or hole bands electronically accessible. Here we demonstrate the first real-space microscopic identification of each termination with a multi-technique experimental approach. Using spatially resolved tunnelling spectroscopy across the lateral boundary between the two terminations, a previously speculated on p-n junction-like discontinuity in electronic structure at the lateral boundary is confirmed experimentally. These findings realize an important step towards the exploitation of the unique behaviour of the Rashba semiconductor BiTeI for new device concepts in spintronics.

Crystal growth of Dirac semimetal ZrSiS with high magnetoresistance and mobility

High quality single crystal ZrSiS as a theoretically predicted Dirac semimetal has been grown successfully using a vapor phase transport method. The single crystals of tetragonal structure are easy to cleave into perfect square-shaped pieces due to the van der Waals bonding between the sulfur atoms of the quintuple layers. Physical property measurement results including resistivity, Hall coefficient (RH), and specific heat are reported. The transport and thermodynamic properties suggest a Fermi liquid behavior with two Fermi pockets at low temperatures. At T = 3 K and magnetic field of Hǁc up to 9 Tesla, large magneto-resistance up to 8500% and 7200% for Iǁ(100) and Iǁ(110) were found. Shubnikov de Haas (SdH) oscillations were identified from the resistivity data, revealing the existence of two Fermi pockets at the Fermi level via the fast Fourier transform (FFT) analysis. The Hall coefficient (RH) showed hole-dominated carriers with a high mobility of 3.05 × 104 cm2 V−1 s−1 at 3 K. ZrSiS has been confirmed to be a Dirac semimetal by the Dirac cone mapping near the X-point via angle resolved photoemission spectroscopy (ARPES) with a Dirac nodal line near the Fermi level identified using scanning tunneling spectroscopy (STS).

Organic Monolayer Protected Topological Surface State.

Perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA)/Bi2Se3 and Fe/PTCDA/Bi2Se3 heterointerfaces are investigated using scanning tunneling microscopy and spectroscopy. The close-packed self-assembled PTCDA monolayer possesses big molecular band gap and weak molecule-substrate interactions, which leaves the Bi2Se3 topological surface state intact under PTCDA. Formation of Fe-PTCDA hybrids removes interactions between the Fe dopant and the Bi2Se3 surface, such as doping effects and Coulomb scattering. Our findings reveal the functionality of PTCDA to prevent dopant disturbances in the TSS and provide an effective alternative for interface designs of realistic TI devices.

Room temperature agglomeration for the growth of BiTeI single crystals with a giant Rashba effect

We report a room temperature agglomeration (RTA) procedure to grow highly homogeneous and impurity-free BiTeI single crystals safely. The proposed four-step procedure of mixing and heating is able to prevent severe iodine loss and avoid the danger of explosion during large scale crystal growth. Following the RTA treatment of the precursor, the single crystals obtained from three different growth methods, including vertical Bridgman, melt growth and chemical vapour transport (CVT), were compared. Crystals grown using the Bridgman method showed the highest residual-resistance ratio (RRR) and mobility, and the largest domain size among the three. The crystal quality and purity have been confirmed using X-ray diffraction, Electron Probe Microanalysis (EPMA), resistivity, TEM, and STM. Additionally, Mn-intercalated and -substituted BiTeI crystals have also been investigated.

In situ magnetization switching of magnetic probes applied to spin-polarized scanning tunneling microscopy

Soft magnetic tip was utilized to be the probe of spin-polarized scanning tunneling microscopy. It was demonstrated that the spin contrast can be reversed by in situ switching tip magnetization through varying tip-substrate distance for resolving perpendicular magnetic domain images. With this in situ magnetization direction switching of the soft magnetic tip, it is conceivable to separate magnetic from chemical and topographic contributions without applying external magnetic field. This provides an effective tool for the study of complex magnetic spin structures with various nonmagnetic impurities or compositions involved.

Moiré-related in-gap states in a twisted MoS 2 /graphite heterojunction

This report presents a series of low-temperature (4.5 K) scanning tunneling microscopy and spectroscopy experimental results on monolayer MoS2 deposited on highly oriented pyrolytic graphite using chemical vapor deposition. To reveal the detailed connection between atomic morphology and conductivity in twisted MoS2/graphite heterojunctions, we employ high-sensitivity tunneling spectroscopy measurements by choosing a reduced tip-sample distance. We discern previously unobserved conductance peaks within the band gap range of MoS2, and by comparing the tunneling spectra from MoS2 grains of varying rotation with respect to the substrate, show that these features have small but non-negligible dependence on the moiré superstructure. Furthermore, within a single moiré supercell, atomically resolved tunneling spectroscopy measurements show that the spectra between the moiré high and low areas are also distinct. These in-gap states are shown to have an energy shift attributed to their local lattice strain, matching corresponding behavior of the conduction band edge, and we therefore infer that these features are intrinsic to the density of states, rather than experimental artifacts, and attribute them to the twisted stacking and local strain energy of the MoS2/graphite heterointerface.Heterointerfaces: Gap states in a twisted heterojunctionNew moiré-related states emerge in the bandgap of molybdenum disulfide when interfaced with highly oriented pyrolytic graphite. Two-dimensional materials enable designer heterostructures to be created layer-by-layer, but greater understanding of how different interfaces affect the electronic structure is required if they are to be fully exploited for applications. An international team of researchers led by Minn-Tsong Lin from National Taiwan University use low-temperature scanning tunneling microscopy and spectroscopy to show that in-gap states can form at molybdenum disulfide/graphite heterointerfaces, which are sensitive to both the stacking angle and local strain, and have a small dependence on the moiré superstructure. These tunable in-gap states, which are attributed to interlayer charges, show the complexity, but also potential of using stacking and strain for engineering the electronic structure of heterostructures.

Quasiparticle Scattering in the Rashba Semiconductor BiTeBr: The Roles of Spin and Defect Lattice Site

Observations of quasiparticle interference have been used in recent years to examine exotic carrier behavior at the surfaces of emergent materials, connecting carrier dispersion and scattering dynamics to real-space features with atomic resolution. We observe quasiparticle interference in the strongly Rashba split 2DEG-like surface band found at the tellurium termination of BiTeBr and examine two mechanisms governing quasiparticle scattering: We confirm the suppression of spin-flip scattering by comparing measured quasiparticle interference with a spin-dependent elastic scattering model applied to the calculated spectral function. We also use atomically resolved STM maps to identify point defect lattice sites and spectro-microscopy imaging to discern their varying scattering strengths, which we understand in terms of the calculated orbital characteristics of the surface band. Defects on the Bi sublattice cause the strongest scattering of the predominantly Bi 6p derived surface band, with other defects causing nearly no scattering near the conduction band minimum.