NH 3 -assisted chloride flux-coating method for direct fabrication of visible-light-responsive SrNbO 2 N crystal layers
SrNbO 2 N crystal layers were prepared on niobium substrates by using an NH 3 -assisted chloride flux-coating method.
Chemistry↗
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Electrically Pumped Epitaxially Regrown GaSb-Based Type-I Quantum-Well Surface-Emitting Lasers with Buried High-Index-Contrast Photonic Crystal Layer
Epitaxially regrown electrically pumped photonic crystal surface-emitting lasers (PCSELs) emitting near 2 and 2.6 μm are designed, fabricated, and characterized. A high-index-contrast photonic crystal layer is incorporated into the GaSb-based laser heterostructure by air-hole-retaining epitaxial regrowth. A square lattice of triangular holes is etched in the top waveguide core layer of the incomplete laser heterostructure. The nanopatterned surface is subsequently cleaned and regrown with AlGaAsSb p-cladding material. Transmission electron microscopy studies demonstrate uniform regrowth over the nanopatterned GaSb surface. The selected regrowth regimes yield a buried 2D array of elongated air-holes. The diode PCSELs based on moderately etched nanopatterns demonstrate band-edge lasing near 2 μm up to room temperatures. The cascade diode PCSELs operate near 2.6 μm with minimum threshold current densities of about 500 A cm -2 achieved at 180 K. The devices generate mW level output in narrow divergence beam emitted from the window in substrate contact. The angle-resolved electroluminescence measurements reveal a four-sub-band band structure with an apparent photonic bandgap corresponding to the buried high-index-contrast square photonic crystal layer. Finally, the PCSELs made of heterostructures supporting two modes in the vertical direction demonstrate two sets of sub-bands showing anti-crossing-like interaction.
77 NANOSCIENCE AND NANOTECHNOLOGY↗
GaSb-based heterostructure with buried vacuum pocket photonic crystal layer
The vacuum pocket retaining molecular beam epitaxial regrowth of the nano-patterned GaSb surface was demonstrated. The high contrast 2D photonic crystal layer was incorporated into the test 2 μm emitting laser heterostructure. The photonic dispersion determined from angle-resolved electroluminescence experiment showed four well-resolved bands corresponding to the model predictions for the square lattice. The single-mode lasing near 2 μm has been observed at the temperature corresponding to the alignment of the photonic crystal band-edge states and the quantum well gain peak. The reference devices without the photonic crystal layer emitted trivial spectra and did not lase at any temperature.
77 NANOSCIENCE AND NANOTECHNOLOGY↗
Wrap–Around Core–Shell Heterostructures of Layered Crystals
Engineered heterostructures create new functionality by integrating dissimilar materials. Combining different 2D crystals naturally produces two distinct classes of heterostructures, vertical van der Waals (vdW) stacks or 2D sheets bonded laterally by covalent line interfaces. Here, when joining thicker layered crystals, the arising structural and topological conflicts can result in more complex geometries. Phase separation during one–pot synthesis of layered tin chalcogenides spontaneously creates core–shell structures in which large orthorhombic SnS crystals are enclosed in a wrap–around shell of trigonal SnS 2 , forcing the coexistence of parallel vdW layering along with unconventional, orthogonally layered core–shell interfaces. Measurements of the optoelectronic properties establish anisotropic carrier separation near type II core–shell interfaces and extended long–wavelength light harvesting via spatially indirect interfacial absorption, making multifunctional layered core–shell structures attractive for energy–conversion applications.
36 MATERIALS SCIENCE↗
Selective-area growth and magnetic characterization of MnAs/AlGaAs nanoclusters on insulating Al{sub 2}O{sub 3} layers crystallized on Si(111) substrates
We report on selective-area metal-organic vapor phase epitaxy and magnetic characterization of coupled MnAs/AlGaAs nanoclusters formed on thin Al{sub 2}O{sub 3} insulating layers crystallized on Si(111) substrates. Cross-sectional transmission electron microscopy reveals that poly-crystalline γ-Al{sub 2}O{sub 3} grains are formed after an annealing treatment of the amorphous Al{sub 2}O{sub 3} layers deposited by atomic layer deposition on Si(111) substrates. The 〈111〉 direction of the γ-Al{sub 2}O{sub 3} grains tends to be oriented approximately parallel to the 〈111〉 direction of the Si substrate. We observe that hexagonal MnAs nanoclusters on AlGaAs buffer layers grown by selective-area metal-organic vapor phase epitaxy on partially SiO{sub 2}-masked Al{sub 2}O{sub 3} insulator crystallized on Si(111) substrates are oriented with the c-axis along the 〈111〉 direction of the substrates, but exhibit a random in-plane orientation. A likely reason is the random orientation of the poly-crystalline γ-Al{sub 2}O{sub 3} grains in the Al{sub 2}O{sub 3} layer plane. Magnetic force microscopy studies at room temperature reveal that arrangements of coupled MnAs nanoclusters exhibit a complex magnetic domain structure. Such arrangements of coupled MnAs nanoclusters may also show magnetic random telegraph noise, i.e., jumps between two discrete resistance levels, in a certain temperature range, which can be explained by thermally activated changes of the complex magnetic structure of the nanocluster arrangements.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
2D photonic crystal layer assisted thiosilicate ceramic plate with red-emitting film for high quality w -LEDs
In this work, we have succeeded in obtaining high quality warm w-light-emitting-diodes (LEDs) by adopting hybrid two-dimensional (2D) structure of SiNx photonic crystal layer (PCL) assisted cyan-emitting ceramic-plate thiosilicate SrLa2Si2S8:Ce3+ with red-emitting film SrLiAl3N4:Eu2+ phosphor on a 430 nm blue LED chip at 350 mA. 2D SiNx PCL was capped with thiosilicate is because it can enhance the luminous efficacy and maintain the low correlated color temperature (CCT) and high color-rendering index (CRI). High luminous efficacy (82.3 lm/W), high special CRI (R9=75) as well as the low CCT (5431 K) of the optimal w-LED was obtained due to the assistances of 2D SiNx PCL and narrow-band red-emitting phosphor with the doping percentage at 10 wt%. The synthesis processes, structural analysis, optical properties and LED device performances were detailed investigated to find out the relationship between the optimum composition and good optical properties. Based on intriguing luminescence properties by the 2D SiNx PCL and red-emitting film phosphor introducing, we proclaim this method could also have high potential application in other phosphor-converted w-LEDs.
36 MATERIALS SCIENCE↗
Hot Carrier and Surface Recombination Dynamics in Layered InSe Crystals
Layered indium selenide (InSe) is a van der Waals solid that has emerged as a promising material for high-performance ultrathin solar cells. The optoelectronic parameters that are critical to photoconversion efficiencies, such as hot carrier lifetime and surface recombination velocity, are however largely unexplored in InSe. Here, these key photophysical properties of layered InSe are measured with femtosecond transient reflection spectroscopy. The hot carrier cooling process is found to occur through phonon scattering. The surface recombination velocity and ambipolar diffusion coefficient are extracted from fits to the pump energy-dependent transient reflection kinetics using a free carrier diffusion model. The extracted surface recombination velocity is approximately an order of magnitude larger than that for methylammonium lead-iodide perovskites, suggesting that surface recombination is a principal source of photocarrier loss in InSe. The extracted ambipolar diffusion coefficient is consistent with previously reported values of InSe carrier mobility.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Cation–Eutectic Transition via Sublattice Melting in CuInP 2 S 6 /In 4/3 P 2 S 6 van der Waals Layered Crystals
Single crystals of the van der Waals layered ferrielectric material CuInP 2 S 6 spontaneously phase separate when synthesized with Cu deficiency. In this paper, we identify a route to form and tune intralayer heterostructures between the corresponding ferrielectric (CuInP 2 S 6 ) and paraelectric (In 4/3 P 2 S 6 ) phases through control of chemical phase separation. We conclusively demonstrate that Cu-deficient Cu 1–x In 1+x/3 P 2 S 6 forms a single phase at high temperature. We also identify the mechanism by which the phase separation proceeds upon cooling. Above 500 K both Cu + and In 3+ become mobile, while P 2 S 6 4– anions maintain their structure. We therefore propose that this transition can be understood as eutectic melting on the cation sublattice. Such a model suggests that the transition temperature for the melting process is relatively low because it requires only a partial reorganization of the crystal lattice. As a result, varying the cooling rate through the phase transition controls the lateral extent of chemical domains over several decades in size. At the fastest cooling rate, the dimensional confinement of the ferrielectric CuInP 2 S 6 phase to nanoscale dimensions suppresses ferrielectric ordering due to the intrinsic ferroelectric size effect. Finally, intralayer heterostructures can be formed, destroyed, and re-formed by thermal cycling, thus enabling the possibility of finely tuned ferroic structures that can potentially be optimized for specific device architectures.
2D ferrielectric↗
Gigahertz Frequency Antiferromagnetic Resonance and Strong Magnon-Magnon Coupling in the Layered Crystal CrCl 3
We report broadband microwave absorption spectroscopy of the layered antiferromagnet CrCl 3 . We observe a rich structure of resonances arising from quasi-two-dimensional antiferromagnetic dynamics. Because of the weak interlayer magnetic coupling in this material, we are able to observe both optical and acoustic branches of antiferromagnetic resonance in the GHz frequency range and a symmetry-protected crossing between them. Furthermore, by breaking rotational symmetry, we further show that strong magnon-magnon coupling with large tunable gaps can be induced between the two resonant modes.
2-dimensional systems↗
A perspective on single-crystal layered oxide cathodes for lithium-ion batteries
As the demand for lithium-ion batteries grows exponentially to feed the nascent electric-vehicle and grid-storage markets, the need for higher energy density and longer cycle life becomes more apparent. Increasing the nickel content in the layered-oxide cathodes has been a dominant strategy to increase energy density, but this has exacerbated the surface reactivity concerns. Furthermore, the high states of charge associated with increased capacity lead to cracking of the polycrystalline cathode particles, which exposes fresh surfaces and accelerates capacity fade. Single-crystal cathode particles with low susceptibility to cracking have recently taken on intense interest due to their remarkable cyclability. Many different approaches to single-crystal synthesis have been explored, but there has been no systematic analysis of the different techniques to date. Additionally, many reports have taken on a trial-and-error approach, ignoring well established literature on grain growth outside the battery field. This perspective reviews the literature on single-crystal cathode synthesis through the lens of classic grain growth theories, providing insight and hopefully accelerating the adoption of the promising single-crystal cathode morphology.
25 ENERGY STORAGE↗
Formation of Cu{sub 2}O and ZnO Crystal Layers by Magnetron Assisted Sputtering and Their Optical Characterization
Copper (I) oxide and zinc oxide films are formed on silicon and glassy quartz substrates by magnetron assisted sputtering. The thickness of the films is tens and hundreds of nanometers. The films are grown at different substrate temperatures and different oxygen pressures in the working chamber. The film samples are studied by the X-ray diffraction technique, scanning electron microscopy, and optical methods. It is established that an increase in the substrate temperature yields a change in the surface morphology of copper (I) oxide films towards the formation of well-pronounced crystallites. The reflectance and Raman spectra suggest that the quality of such films is close to that of bulk Cu{sub 2}O crystals produced by the oxidation of copper. As concerns ZnO films, an increase in the substrate temperature and an increase in the partial oxygen pressure make it possible to produce films, for which a sharp exciton structure is observed in the reflectance spectra and the emission of excitons bound at donors is observed in the luminescence spectra.
36 MATERIALS SCIENCE↗
Quasi-layered Crystal Structure Coupled with Point Defects Leading to Ultralow Lattice Thermal Condu
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Ye, Zhengyang↗
Multiphonon diffuse scattering in solids from first principles: Application to layered crystals and two-dimensional materials
Time-resolved diffuse scattering experiments have gained increasing attention due to their potential to reveal nonequilibrium dynamics of crystal lattice vibrations with full momentum resolution. Although progress has been made in interpreting experimental data on the basis of one-phonon scattering, understanding the role of individual phonons can be sometimes hindered by multiphonon excitations. In Ref. [M. Zacharias, H. Seiler, F. Caruso, D. Zahn, F. Giustino, P. C. Kelires, and R. Ernstorfer, Phys. Rev. Lett. 127, 207401 (2021)], we have introduced a rigorous approach for the calculation of the all-phonon inelastic scattering intensity of solids from first-principles. In the present work, we describe our implementation in detail and show that multiphonon interactions are captured efficiently by exploiting translational and time-reversal symmetries of the crystal. We demonstrate its predictive power by calculating the scattering patterns of monolayer molybdenum disulfide (MoS 2 ), bulk MoS 2 , and black phosphorus (bP), and we obtain excellent agreement with our measurements of thermal electron diffuse scattering. Remarkably, our results show that multiphonon excitations dominate in bP across multiple Brillouin zones, while in MoS 2 they play a less pronounced role. We expand our analysis for each system and examine the effect of individual atomic and interatomic vibrational motion on the diffuse scattering signals. We further demonstrate the high-throughput capability of our approach by reporting all-phonon scattering maps of two-dimensional MoSe 2 , WSe 2 , WS 2 , graphene, and CdI 2 , rationalizing in each case the effect of multiphonon processes. As a side point, we show that the special displacement method reproduces the thermally distorted configuration that generates precisely the all-phonon diffuse pattern. In conclusion, the present methodology opens the way for systematic calculations of the scattering intensity in crystals and the accurate interpretation of static and time-resolved inelastic scattering experiments.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Transport properties and crystal structure of layered LaSb 2
LaSb 2 has a layered crystal structure along the c-axis with ~2% difference between the in-plane orthorombic a and b axes. Here, we report on the thermal conductivity, electrical resistivity, and Seebeck coefficient from 10 to 300 K as well as the magnetoresistance at 10 K. Using the van der Pauw technique on single crystal samples, the in-plane electrical resistivity tensor has been measured and it is found to be isotropic. An anisotropic crystal structure may have isotropic properties, but in the present case, the isotropic nature stems from crystal imperfection. Single crystal X-ray diffraction provides evidence of a mixing of the in-plane a- and b-directions leading to observed diffraction intensity where systematic absences are expected. Whether the underlying structural mechanism is twinning or stacking faults is unknown, but it could be the origin of the previously observed charge density wave states, and it may also explain the high unsaturating linear magnetoresistance reported here. At ambient conditions, LaSb 2 is found to be stable in air, with no sign of bulk degradation after 5 years of storage; however, some change is observed in the amorphous background scattering.
36 MATERIALS SCIENCE↗
Stepwise crystallization and the layered distribution in crystallization kinetics of ultra-thin poly(ethylene terephthalate) film
Crystallization is an important property of polymeric materials. In conventional viewpoint, the transformation of disordered chains into crystals is usually a spatially homogeneous process (i.e., it occurs simultaneously throughout the sample), that is, the crystallization rate at each local position within the sample is almost the same. Here, we show that crystallization of ultra-thin poly(ethylene terephthalate) (PET) films can occur in the heterogeneous way, exhibiting a stepwise crystallization process. We found that the layered distribution of glass transition dynamics of thin film modifies the corresponding crystallization behavior, giving rise to the layered distribution of the crystallization kinetics of PET films, with an 11-nm-thick surface layer having faster crystallization rate and the underlying layer showing bulk-like behavior. The layered distribution in crystallization kinetics results in a particular stepwise crystallization behavior during heating the sample, with the two cold-crystallization temperatures separated by up to 20 K. Meanwhile, interfacial interaction is crucial for the occurrence of the heterogeneous crystallization, as the thin film crystallizes simultaneously if the interfacial interaction is relatively strong. We anticipate that this mechanism of stepwise crystallization of thin polymeric films will allow new insight into the chain organization in confined environments and permit independent manipulation of localized properties of nanomaterials.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Single-crystal-like GdNdO{sub x} thin films on silicon substrates by magnetron sputtering and high-temperature annealing for crystal seed layer application
Single-crystal-like rare earth oxide thin films on silicon (Si) substrates were fabricated by magnetron sputtering and high-temperature annealing processes. A 30-nm-thick high-quality GdNdO{sub x} (GNO) film was deposited using a high-temperature sputtering process at 500°C. A Gd{sub 2}O{sub 3} and Nd{sub 2}O{sub 3} mixture was used as the sputtering target, in which the proportions of Gd{sub 2}O{sub 3} and Nd{sub 2}O{sub 3} were controlled to make the GNO’s lattice parameter match that of the Si substrate. To further improve the quality of the GNO film, a post-deposition annealing process was performed at a temperature of 1000°C. The GNO films exhibited a strong preferred orientation on the Si substrate. In addition, an Al/GNO/Si capacitor was fabricated to evaluate the dielectric constant and leakage current of the GNO films. It was determined that the single-crystal-like GNO films on the Si substrates have potential for use as an insulator layer for semiconductor-on-insulator and semiconductor/insulator multilayer applications.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Soliton-like defects in nematic liquid crystal thin layers
The nonsingular soliton-like defects in plane nematic liquid crystal (NLC) layers and spherical NLC drops are experimentally detected and studied when the interaction of NLC molecules with a bounding surface is varied. The dynamics and the annihilation of nonsingular defects of opposite signs on a plane surface are investigated. Periodic transformations of the soliton-like defects in NLC drops in an electric field are detected. The theory of elasticity is used to show that the surface energy taken into account in the total free energy of NLC in the case of weak anchoring leads to the possibility of nonsingular solutions of a director equilibrium equation. The calculated pictures of director distribution in a plane NLC layer and in a spherical NLC drop characterized by weak surface anchoring agree well with the results of polarized light optical observations.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗