High-quality Single-crystalline Research Articles

Epitaxial growth of cubic silicon carbide on silicon using hot filament chemical vapor deposition

We are reporting the application of hot filament chemical vapor deposition for the growth of high-quality single-crystalline cubic silicon carbide heteroepitaxially on silicon substrates. Rocking curve X-ray diffraction measurements revealed a full-width at half maximum as low as 333arcsec for a 15μm thick layer. Low tensile strain, below 0.1%, was measured using Raman spectroscopy resulting in a wafer bow as low as 6μm over a full 4″ substrate. We achieved this quality using a carefully optimized process making use of the additional degrees of freedom the hot filaments create. These allow for precursor pre-cracking and a tuning of the vertical thermal gradient, which creates an improved thermal field compared to classic chemical vapor deposition techniques used for the deposition of this material today. Measurements of the material uniformity show an influence of the lateral temperature field and of the stoichiometry, which is influenced by the graphite based sample holder.

Superconductivity and magnetotransport of single-crystalline NbSe2 nanoplates grown by chemical vapour deposition.

NbSe2 is a typical transition metal dichalcogenide with a rich variety of electronic ground states existing in its nanostructures, including two-dimensional superconductivity and charge density wave. However, the direct growth of high-quality single-crystalline NbSe2 nanostructures is still challenging, which limits their applications in electronic devices. Here, we report the growth of high-quality NbSe2 nanoplates by a single-step chemical vapour deposition. Their temperature and magnetic-field dependent superconducting behaviors were investigated by four-terminal devices fabricated on individual nanostructures. The NbSe2 nanoplates show two-dimensional characteristics of superconducting transitions and strong anisotropy with magnetic field orientation, providing potential platforms for the exploration of new physics in nanoelectronic devices.

Edge-Controlled Growth and Etching of Two-Dimensional GaSe Monolayers.

Understanding the atomistic mechanisms governing the growth of two-dimensional (2D) materials is of great importance in guiding the synthesis of wafer-sized, single-crystalline, high-quality 2D crystals and heterostructures. Etching, in many cases regarded as the reverse process of material growth, has been used to study the growth kinetics of graphene. In this work, we explore a growth-etching-regrowth process of monolayer GaSe crystals, including single-crystalline triangles and irregularly shaped domains formed by merged triangles. We show that the etching begins at a slow rate, creating triangular, truncated triangular, or hexagonally shaped holes that eventually evolve to exclusively triangles that are rotated 60° with respect to the crystalline orientation of the monolayer triangular crystals. The regrowth occurs much faster than etching, reversibly filling the etched holes and then enlarging the size of the monolayer crystals. A theoretical model developed based on kinetic Wulff construction (KWC) theory and density functional theory (DFT) calculations accurately describe the observed morphology evolution of the monolayer GaSe crystals and etched holes during the growth and etching processes, showing that they are governed by the probability of atom attachment/detachment to/from different types of edges with different formation energies of nucleus/dents mediated by chemical potential difference Δμ between Ga and Se. Our growth-etching-regrowth study provides not only guidance to understand the growth mechanisms of 2D binary crystals but also a potential method for the synthesis of large, shape-controllable, high-quality single-crystalline 2D crystals and their lateral heterostructures.

High-Quality Bi2Te3 Single Crystalline Films on Flexible Substrates and Bendable Photodetectors**Supported by the National Basic Research Program of China under Grant No 2012CB619200, the National Natural Science Foundation of China under Grant Nos 61290304, 11074265 and 11174307, the Natural Science Foundation of Shanghai under Grant No 16ZR1441200, and the Frontier Science Research Project (Key Programs) of Chinese Academy of Sciences

Recently, great efforts have been made in the fabrication of arbitrary warped devices to satisfy the requirement of wearable and lightweight electronic products. Direct growth of high crystalline quality films on flexible substrates is the most desirable method to fabricate flexible devices owing to the advantage of simple and compatible preparation technology with current semiconductor devices, while it is a very challenging work, and usually amorphous, polycrystalline or discontinuous single crystalline films are achieved. Here we demonstrate the direct growth of high-quality Bi2Te3 single crystalline films on flexible polyimide substrates by the modified hot wall epitaxy technique. Experimental results reveal that adjacent crystallites are coherently coalesced to form a continuous film, although amounts of disoriented crystallites are generated due to fast growth rate. By inserting a quartz filter into the growth tube, the number density of disoriented crystallites is effectively reduced owing to the improved spiral interaction. Furthermore, flexible Bi2 Te3 photoconductors are fabricated and exhibit strong near-infrared photoconductive response under different degrees of bending, which also confirms the obtained flexible films suitable for electronic applications.

SANS study of vortex lattice structural transition in optimally doped (Ba1−xKx)Fe2As2

Small-angle neutron scattering on high quality single crystalline Ba1−xKxFe2As2 reveals the transition from a low-field vortex solid phase with orientational order to a vortex polycrystal at high magnetic field. The vortex order–disorder transition is correlated with the second-peak feature in isothermal hysteresis loops, and is interpreted in terms of the generation of supplementary vortex solid dislocations. The sharp drop of the structure factor above the second peak field is explained by the dynamics of freezing of the vortex ensemble in the high field phase.

Fabrications and application of single crystalline GaN for high-performance deep UV photodetectors

High-quality single crystalline Gallium Nitride (GaN) semiconductor has been synthesized using molecule beam epitaxy (MBE) technique for development of high-performance deep ultraviolet (UV) photodetectors. Thickness of the films was estimated by using surface profile meter and scanning electron microscope. Electronic states and elemental composition of the films were obtained using Raman scattering spectroscopy. The orientation, crystal structure and phase purity of the films were examined using a Siemens x-ray diffractometer radiation. The surface microstructure was studied using high resolution scanning electron microscopy (SEM). Two types of metal pairs: Al-Al, Al-Cu or Cu-Cu were used for interdigital electrodes on GaN film in order to examine the Schottky properties of the GaN based photodetector. The characterizations of the fabricated prototype include the stability, responsivity, response and recovery times. Typical time dependent photoresponsivity by switching different UV light source on and off five times for each 240 seconds at a bias of 2V, respectively, have been obtained. The detector appears to be highly sensitive to various UV wavelengths of light with very stable baseline and repeatability. The obtained photoresponsivity was up to 354 mA/W at the bias 2V. Higher photoresponsivity could be obtained if higher bias was applied but it would unavoidably result in a higher dark current. Thermal effect on the fabricated GaN based prototype was discussed.

2D layered transport properties from topological insulator Bi2Se3 single crystals and micro flakes.

Low-field magnetotransport measurements of topological insulators such as Bi2Se3 are important for revealing the nature of topological surface states by quantum corrections to the conductivity, such as weak-antilocalization. Recently, a rich variety of high-field magnetotransport properties in the regime of high electron densities (∼1019 cm−3) were reported, which can be related to additional two-dimensional layered conductivity, hampering the identification of the topological surface states. Here, we report that quantum corrections to the electronic conduction are dominated by the surface states for a semiconducting case, which can be analyzed by the Hikami-Larkin-Nagaoka model for two coupled surfaces in the case of strong spin-orbit interaction. However, in the metallic-like case this analysis fails and additional two-dimensional contributions need to be accounted for. Shubnikov-de Haas oscillations and quantized Hall resistance prove as strong indications for the two-dimensional layered metallic behavior. Temperature-dependent magnetotransport properties of high-quality Bi2Se3 single crystalline exfoliated macro and micro flakes are combined with high resolution transmission electron microscopy and energy-dispersive x-ray spectroscopy, confirming the structure and stoichiometry. Angle-resolved photoemission spectroscopy proves a single-Dirac-cone surface state and a well-defined bulk band gap in topological insulating state. Spatially resolved core-level photoelectron microscopy demonstrates the surface stability.

Insulator-to-metal transition in vanadium supersaturated silicon: variable-range hopping and Kondo effect signatures

We report the observation of the insulator-to-metal transition in crystalline silicon samples supersaturated with vanadium. Ion implantation followed by pulsed laser melting and rapid resolidification produce high quality single-crystalline silicon samples with vanadium concentrations that exceed equilibrium values in more than 5 orders of magnitude. Temperature-dependent analysis of the conductivity and Hall mobility values for temperatures from 10 K to 300 K indicate that a transition from an insulating to a metallic phase is obtained at a vanadium concentration between 1.1 × 1020 and 1.3 × 1021 cm−3. Samples in the insulating phase present a variable-range hopping transport mechanism with a Coulomb gap at the Fermi energy level. Electron wavefunction localization length increases from 61 to 82 nm as the vanadium concentration increases in the films, supporting the theory of impurity band merging from delocalization of levels states. On the metallic phase, electronic transport present a dispersion mechanism related with the Kondo effect, suggesting the presence of local magnetic moments in the vanadium supersaturated silicon material.

ChemInform Abstract: Multiferroic Hexagonal Ferrites (h‐RFeO3, R: Y, Dy‐Lu): A Brief Experimental Review

AbstractReview: 88 refs.

Characteristics of TlBr single crystals grown using the vertical Bridgman-Stockbarger method for semiconductor-based radiation detector applications

AbstractTlBr single crystals grown using the vertical Bridgman-Stockbarger method were characterized for semiconductor based radiation detector applications. It has been shown that the vertical Bridgman-Stockbarger method is effective to grow high-quality single crystalline ingots of TlBr. The TlBr single crystalline sample, which was located 6 cm from the tip of the ingot, exhibited lower impurity concentration, higher crystalline quality, high enough bandgap (>2.7 eV), and higher resistivity (2.5 × 1011Ω·cm) which enables using the fabricated samples from the middle part of the TlBr ingot for fabricating high performance semiconductor radiation detectors.

Large-scale synthesis and electrical transport properties of single-crystalline SmB6 nanowires

Topological Kondo insulator samarium hexaboride (SmB6) nanowires, with diameters of 60–150 nm and lengths up to 1–5 μm, were successfully synthesized in large scale by chemical vapor deposition using BCl3 and SmCl3 as precursors at 1070 °C. Transmission electron microscopy observation and selected area electron diffraction analysis indicate that SmB6 nanowires are single-crystalline and grow in a preferred direction of [1 0 0]. It also indicates that the growth of SmB6 nanowires might be governed by a vapor–solid mechanism. Conventional four-terminal resistance measurements show that the resistance of an SmB6 nanowire increases with decreasing temperature, but saturates at temperatures less than 10 K, which might be attributed to a true topological insulator with a metallic surface and fully insulating bulk states. Resistance measurements also indicate that the contribution of surface states to conductance in the SmB6 nanowire is enhanced remarkably; therefore the high-quality single-crystalline SmB6 nanowires with large surface-to-bulk ratio might be the best candidate for investigating the topological properties of this material.

Photophysical and electrical properties of organic waveguide nanorods of perylene-3,4,9,10-tetracarboxylic dianhydride

The single crystalline nanostructure of organic semiconductors provides a very promising class of materials for applications in modern optoelectronic devices. However, morphology control and optoelectronic property modulation of high quality single crystalline samples remain a challenge. Here, we report the morphology-controlled growth of single crystalline nanorod arrays of perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA). We demonstrate that, unlike PTCDA film, PTCDA nanorods exhibits optical waveguide features, enhanced absorption, and Frenkel excitation emission in the visible region. Additionally, we measured the electrical properties of PTCDA nanorods, including the conductivity along the growth direction of the nanorod, which is roughly 0.61 S·m–1 (much higher than that of pure crystalline PTCDA films).

Nodeless superconductivity in the noncentrosymmetric superconductor BiPd

We report low-temperature thermal conductivity measurements on high-quality single crystalline α-BiPd, a noncentrosymmetric superconductor with Tc ≃ 3.8 K. In zero magnetic field, the residual linear term κ0/T is absent, indicating a full gap and suggesting dominant singlet pairing. Consistent with this picture, κ0(H)/T shows weak field dependence in low field, but grows relatively fast in fields above 0.03 T (≃1/5Hc2). Implications for the material’s disputed high-field behavior are discussed, and constraints are placed on the previously proposed scenarios.

A new approach for fabrications of SiC based photodetectors.

We report on a new approach to quickly synthesize high-quality single crystalline wide band gap silicon carbide (SiC) films for development of high-performance deep ultraviolet (UV) photodetectors. The fabricated SiC based UV photodetectors exhibited high response while maintaining cost-effectiveness and size miniaturization. Focus of the experiments was on studies of electrical and electronic properties, as well as responsivity, response and recovery times, and repeatability of the deep UV photodetectors. Raman scattering spectroscopy and scanning electron microscope (SEM) were used to characterize the SiC materials. Analyses of the SEM data indicated that highly flat SiC thin films have been obtained. Based on the synthesized SiC, deep UV detectors are designed, fabricated, and tested with various UV wavelength lights at different radiation intensities. Temperature effect and bias effect on the photocurrent strength and signal-to-noise ratio, humidity effect on the response time and recovery time of the fabricated detectors have been carefully characterized and discussed. The detectors appear to have a very stable baseline and repeatability. The obtained responsivity is more than 40% higher compared to commercial detectors. The good performance of the photodetectors at operating temperature up to 300 °C remains nearly unchanged.

Enhanced thermoelectric properties of topological crystalline insulator PbSnTe nanowires grown by vapor transport

Bulk PbTe and alloy compounds thereof are well-known thermoelectric materials for electric power generation. Among these alloys, PbSnTe hosts unique topological surface states that may have improved thermoelectric properties. Here we report on the vapor-transport growth and thermoelectric study of high-quality single-crystalline PbTe and PbSnTe nanowires. The nanowires were grown along the direction with dominant {100} facets; the chemical compositions of the wires depend strongly on the substrate position in the growth reactor. We measured the thermopower and electrical and thermal conductivities of individual nanowires to determine the thermoelectric figure of merit ZT. Compared to bulk samples, the PbSnTe nanowires showed both improved thermopower and suppressed thermal conductivity, enhancing the ZTs to ~0.018 and ~0.035 at room temperature. The enhanced thermopower may result from the unique topological surface states; the suppression of thermal conductivity may relate to increased phonon-surface scattering. Compared to PbTe nanowires, the PbSnTe wires have lower thermopower but significantly higher electrical conductivities. This study highlights nanostructuring in combination with alloying as an important approach to enhancing the figure of merit ZT of thermoelectric materials.

Free-Standing Two-Dimensional Single-Crystalline InSb Nanosheets.

Growth of high-quality single-crystalline InSb layers remains challenging in material science. Such layered InSb materials are highly desired for searching for and manipulation of Majorana Fermions in solid state, a fundamental research task in physics today, and for development of novel high-speed nanoelectronic and infrared optoelectronic devices. Here, we report on a new route toward growth of single-crystalline, layered InSb materials. We demonstrate the successful growth of free-standing, two-dimensional InSb nanosheets on one-dimensional InAs nanowires by molecular-beam epitaxy. The grown InSb nanosheets are pure zinc-blende single crystals. The length and width of the InSb nanosheets are up to several micrometers and the thickness is down to ∼10 nm. The InSb nanosheets show a clear ambipolar behavior and a high electron mobility. Our work will open up new technology routes toward the development of InSb-based devices for applications in nanoelectronics, optoelectronics, and quantum electronics and for the study of fundamental physical phenomena.

Effect of nitridation surface treatment on silicon (1 1 1) substrate for the growth of high quality single-crystalline GaN hetero-epitaxy layer by MOCVD

A single-crystalline with high quality of gallium nitride epilayers was grown on silicon (111) substrate by metal organic chemical vapor deposition. The process of nitridation surface treatment was accomplished on silicon (111) substrate by flowing the ammonia gaseous. Then, it was followed by a thin aluminum nitride nucleation layer, aluminum nitride/gallium nitride multi-layer and a thick gallium nitride epilayer. The influence of in situ nitridation surface treatment on the crystallinity quality of gallium nitride epilayers was studied by varying the nitridation times at 40, 220 and 400s, respectively. It was shown that the nitridation times greatly affect the structural properties of the grown top gallium nitride epilayer on silicon (111) substrate. In the (0002) and (1 0 1¯ 2) X-ray rocking curve analysis, a narrower value of full width at half-maximum has been obtained as the nitridation time increased. This is signifying the reduction of dislocation density in the gallium nitride epilayer. This result was supported by the value of bowing and root mean square roughness measured by surface profilometer and atomic force microscopy. Furthermore, a crack-free gallium nitride surface with an abrupt cross-sectional structure that observed using field effect scanning electron microscopy was also been obtained. The phi-scan curve of asymmetric gallium nitride proved the top gallium nitride epilayer exhibited a single-crystalline structure.

Ultrathin SnSe2 Flakes Grown by Chemical Vapor Deposition for High-Performance Photodetectors.

High-quality ultrathin single-crystalline SnSe2 flakes are synthesized under atmospheric-pressure chemical vapor deposition for the first time. A high-performance photodetector based on the individual SnSe2 flake demonstrates a high photoresponsivity of 1.1 × 10(3) A W(-1), a high EQE of 2.61 × 10(5)%, and superb detectivity of 1.01 × 10(10) Jones, combined with fast rise and decay times of 14.5 and 8.1 ms, respectively.

Single-Crystalline Thin Films for Studying Intrinsic Properties of BiFeO3–SrTiO3 Solid Solution Photoelectrodes in Solar Energy Conversion

Solid solutions have been widely investigated for solar energy conversion because of the ease to control properties (e.g., band edge positions, charge carrier transport, and chemical stability). In this study, we introduce a new method to investigate intrinsic solar energy conversion properties of solid solutions through fabricating high-quality single-crystalline solid solution films by pulsed laser deposition. This method rules out external factors, such as morphology, crystalline grain size, orientation, density and distribution, surface area, and particle–particle or particle–conducting layer connection, that have plagued previous studies on solid solution photoelectrodes. Perovskite BiFeO3 (BFO) and SrTiO3 (STO) were chosen as “end” members of the solid solutions (i.e., (BFO)x(STO)1–x (0 ≤ x ≤ 1)). Optical and photoelectrochemical (PEC) properties of the solid solutions significantly varied with changing compositions. Among the six studied compositions, BFO:STO (3:1 molar ratio) exhibited the highest...

High-quality EuO thin films the easy way via topotactic transformation.

Epitaxy is widely employed to create highly oriented crystalline films. A less appreciated, but nonetheless powerful means of creating such films is via topotactic transformation, in which a chemical reaction transforms a single crystal of one phase into a single crystal of a different phase, which inherits its orientation from the original crystal. Topotactic reactions may be applied to epitactic films to substitute, add or remove ions to yield epitactic films of different phases. Here we exploit a topotactic reduction reaction to provide a non-ultra-high vacuum (UHV) means of growing highly oriented single crystalline thin films of the easily over-oxidized half-metallic semiconductor europium monoxide (EuO) with a perfection rivalling that of the best films of the same material grown by molecular-beam epitaxy or UHV pulsed-laser deposition. As the technique only requires high-vacuum deposition equipment, it has the potential to drastically improve the accessibility of high-quality single crystalline films of EuO as well as other difficult-to-synthesize compounds.