Showing papers on "Phase (matter) published in 2017"

Structural phase transition in monolayer MoTe 2 driven by electrostatic doping

Abstract: Monolayers of transition-metal dichalcogenides (TMDs) exhibit numerous crystal phases with distinct structures, symmetries and physical properties. Exploring the physics of transitions between these different structural phases in two dimensions may provide a means of switching material properties, with implications for potential applications. Structural phase transitions in TMDs have so far been induced by thermal or chemical means; purely electrostatic control over crystal phases through electrostatic doping was recently proposed as a theoretical possibility, but has not yet been realized. Here we report the experimental demonstration of an electrostatic-doping-driven phase transition between the hexagonal and monoclinic phases of monolayer molybdenum ditelluride (MoTe2). We find that the phase transition shows a hysteretic loop in Raman spectra, and can be reversed by increasing or decreasing the gate voltage. We also combine second-harmonic generation spectroscopy with polarization-resolved Raman spectroscopy to show that the induced monoclinic phase preserves the crystal orientation of the original hexagonal phase. Moreover, this structural phase transition occurs simultaneously across the whole sample. This electrostatic-doping control of structural phase transition opens up new possibilities for developing phase-change devices based on atomically thin membranes.

Origin of Reversible Photoinduced Phase Separation in Hybrid Perovskites.

Abstract: The distinct physical properties of hybrid organic–inorganic materials can lead to unexpected nonequilibrium phenomena that are difficult to characterize due to the broad range of length and time scales involved. For instance, mixed halide hybrid perovskites are promising materials for optoelectronics, yet bulk measurements suggest the halides reversibly phase separate upon photoexcitation. By combining nanoscale imaging and multiscale modeling, we find that the nature of halide demixing in these materials is distinct from macroscopic phase separation. We propose that the localized strain induced by a single photoexcited charge interacting with the soft, ionic lattice is sufficient to promote halide phase separation and nucleate a light-stabilized, low-bandgap, ∼8 nm iodide-rich cluster. The limited extent of this polaron is essential to promote demixing because by contrast bulk strain would simply be relaxed. Photoinduced phase separation is therefore a consequence of the unique electromechanical propert...

Phase engineering of a multiphasic 1T/2H MoS2 catalyst for highly efficient hydrogen evolution

Abstract: Molybdenum disulfide (MoS2) has attracted much attention as a promising electrocatalyst for the hydrogen evolution reaction (HER). Although tremendous efforts have been made to enhance the HER performance of MoS2, the functional design of its intrinsic structures still remains challenging. In this work, a highly active and stable multiphasic catalyst (1T/2H MoS2) is developed through a facile hydrothermal route, in which the 1T phase is induced by the intercalation of guest ions and molecules, and the concentration of the 1T phase can be controlled by adjusting the preparation temperature. The existence of the 1T phase provides more active sites and better conductivity for the HER, resulting in an excellent activity with a small Tafel slope of 46 mV dec−1. More importantly, the integration with the 2H phase is beneficial to the stabilization of the metastable 1T phase, ensuring the excellent durability of 1T/2H MoS2.

Optimized Separation of Acetylene from Carbon Dioxide and Ethylene in a Microporous Material

Abstract: Selective separation of acetylene (C2H2) from carbon dioxide (CO2) or ethylene (C2H4) needs specific porous materials whose pores can realize sieving effects while pore surfaces can differentiate their recognitions for these molecules of similar molecular sizes and physical properties We report a microporous material [Zn(dps)2(SiF6)] (UTSA-300, dps = 4,4′-dipyridylsulfide) with two-dimensional channels of about 33 A, well-matched for the molecular sizes of C2H2 After activation, the network was transformed to its closed-pore phase, UTSA-300a, with dispersed 0D cavities, accompanied by conformation change of the pyridyl ligand and rotation of SiF62– pillars Strong C–H···F and π–π stacking interactions are found in closed-pore UTSA-300a, resulting in shrinkage of the structure Interestingly, UTSA-300a takes up quite a large amounts of acetylene (764 cm3 g–1), while showing complete C2H4 and CO2 exclusion from C2H2 under ambient conditions Neutron powder diffraction and molecular modeling studies clea

From Nonluminescent Cs4PbX6 (X = Cl, Br, I) Nanocrystals to Highly Luminescent CsPbX3 Nanocrystals: Water-Triggered Transformation through a CsX-Stripping Mechanism

Abstract: We report a novel CsX-stripping mechanism that enables the efficient chemical transformation of nonluminescent Cs4PbX6 (X = Cl, Br, I) nanocrystals (NCs) to highly luminescent CsPbX3 NCs. During the transformation, Cs4PbX6 NCs dispersed in a nonpolar solvent are converted into CsPbX3 NCs by stripping CsX through an interfacial reaction with water in a different phase. This process takes advantage of the high solubility of CsX in water as well as the ionic nature and high ion diffusion property of Cs4PbX6 NCs, and produces monodisperse and air-stable CsPbX3 NCs with controllable halide composition, tunable emission wavelength covering the full visible range, narrow emission width, and high photoluminescent quantum yield (up to 75%). An additional advantage is that this is a clean synthesis as Cs4PbX6 NCs are converted into CsPbX3 NCs in the nonpolar phase while the byproduct of CsX is formed in water that could be easily separated from the organic phase. The as-prepared CsPbX3 NCs show enhanced stability a...

Phase transitions in bismuth-modified silver niobate ceramics for high power energy storage

Abstract: Ag(Nb0.8Ta0.2)O3 is used here as a model system to shed light on the nature of the low temperature phase behavior of the unsubstituted parent compound AgNbO3, which is an important material for high-power energy storage applications. The three dielectric anomalies previously identified as M1 ↔ M2, Tf and M2 ↔ M3 transitions in AgNbO3 ceramics are found to be intimately related to the polarization the behavior of the B-site cations. In particular, the M1 ↔ M2 transition is found to involve the disappearance of original ferroelectric polar structure in the M1 phase. Analysis of weak-field and strong field hysteresis loops in the M2 region below Tf suggests the presence of a weakly-polar structure exhibiting antipolar behavior (i.e., a non-compensated antiferroelectric), which can be considered as ferrielectric (FIE). Modeling of the permittivity data using the Curie–Weiss law indicates that the Curie temperature is close to the freezing temperature, Tf, which can be regarded as the Curie point of the FIE phase. Substitution by Ta5+ in this system enhances the stability of the weakly polar/antiferroelectric state, giving rise to an increased energy storage density of 3.7 J cm−3 under an applied field of 27 MV m−1, one of the highest values ever reported for a dielectric ceramic. Furthermore, the energy storage capability remains approximately constant at around 3 J cm−3 up to 100 °C, at an applied field of 22 MV m−1.

Argon Plasma Induced Phase Transition in Monolayer MoS2

Abstract: In this work, we report a facile, clean, controllable and scalable phase engineering technique for monolayer MoS2. We found that weak Ar-plasma bombardment can locally induce 2H→1T phase transition in monolayer MoS2 to form mosaic structures. These 2H→1T phase transitions are stabilized by point defects (single S-vacancies) and the sizes of induced 1T domains are typically a few nanometers, as revealed by scanning tunneling microscopy measurements. On the basis of a selected-area phase patterning process, we fabricated MoS2 FETs inducing 1T phase transition within the metal contact areas, which exhibit substantially improved device performances. Our results open up a new route for phase engineering in monolayer MoS2 and other transition metal dichalcogenide (TMD) materials.

Amorphous nickel-cobalt complexes hybridized with 1T-phase molybdenum disulfide via hydrazine-induced phase transformation for water splitting.

Abstract: Highly active and robust eletcrocatalysts based on earth-abundant elements are desirable to generate hydrogen and oxygen as fuels from water sustainably to replace noble metal materials. Here we report an approach to synthesize porous hybrid nanostructures combining amorphous nickel-cobalt complexes with 1T phase molybdenum disulfide (MoS2) via hydrazine-induced phase transformation for water splitting. The hybrid nanostructures exhibit overpotentials of 70 mV for hydrogen evolution and 235 mV for oxygen evolution at 10 mA cm−2 with long-term stability, which have superior kinetics for hydrogen- and oxygen-evolution with Tafel slope values of 38.1 and 45.7 mV dec−1. Moreover, we achieve 10 mA cm−2 at a low voltage of 1.44 V for 48 h in basic media for overall water splitting. We propose that such performance is likely due to the complete transformation of MoS2 to metallic 1T phase, high porosity and stabilization effect of nickel-cobalt complexes on 1T phase MoS2. Electrocatalysts based on earth-abundant elements have emerged as promising candidates to replace noble metal materials. Here, the authors develop porous hybrid nanostructures combining amorphous Ni-Co complexes with 1T phase MoS2for enhanced electrocatalytic activity for overall water splitting.

Boron‐Dependency of Molybdenum Boride Electrocatalysts for the Hydrogen Evolution Reaction

Abstract: Molybdenum-based materials have been considered as alternative catalysts to noble metals, such as platinum, for the hydrogen evolution reaction (HER). We have synthesized four binary bulk molybdenum borides Mo2 B, α-MoB, β-MoB, and MoB2 by arc-melting. All four phases were tested for their electrocatalytic activity (linear sweep voltammetry) and stability (cyclic voltammetry) with respect to the HER in acidic conditions. Three of these phases were studied for their HER activity and by X-ray photoelectron spectroscopy (XPS) for the first time; MoB2 and β-MoB show excellent activity in the same range as the recently reported α-MoB and β-Mo2 C phases, while the molybdenum richest phase Mo2 B show significantly lower HER activity, indicating a strong boron-dependency of these borides for the HER. In addition, MoB2 and β-MoB show long-term cycle stability in acidic solution.

Observation of extreme phase transition temperatures of water confined inside isolated carbon nanotubes

Abstract: Fluid phase transitions inside single, isolated carbon nanotubes are predicted to deviate substantially from classical thermodynamics. This behaviour enables the study of ice nanotubes and the exploration of their potential applications. Here we report measurements of the phase boundaries of water confined within six isolated carbon nanotubes of different diameters (1.05, 1.06, 1.15, 1.24, 1.44 and 1.52 nm) using Raman spectroscopy. The results reveal an exquisite sensitivity to diameter and substantially larger temperature elevations of the freezing transition (by as much as 100 °C) than have been theoretically predicted. Dynamic water filling and reversible freezing transitions were marked by 2–5 cm−1 shifts in the radial breathing mode frequency, revealing reversible melting bracketed to 105–151 °C and 87–117 °C for 1.05 and 1.06 nm single-walled carbon nanotubes, respectively. Near-ambient phase changes were observed for 1.44 and 1.52 nm nanotubes, bracketed between 15–49 °C and 3–30 °C, respectively, whereas the depression of the freezing point was observed for the 1.15 nm nanotube between −35 and 10 °C. We also find that the interior aqueous phase reversibly decreases the axial thermal conductivity of the nanotube by as much as 500%, allowing digital control of the heat flux. A vibrational spectroscopy technique is used to study vapour, liquid and solid water within isolated carbon nanotubes and reveals phase transitions that show an extreme sensitivity to nanotube diameter, with melting temperatures higher than 100 °C for 1.05 and 1.06 nm diameter nanotubes and below 0 °C for 1.24 and 1.44 nm diameter nanotubes.

Copper-substituted Na0.67Ni0.3−xCuxMn0.7O2 cathode materials for sodium-ion batteries with suppressed P2–O2 phase transition

Abstract: P2-type sodium layered oxides NaxMO2 (M = transition metal) are considered as one kind of promising cathode material for sodium-ion batteries because of their known structures, superior electrochemical properties, and their ease of synthesis. The Ni2+/Ni3+ and Ni3+/Ni4+ redox reactions endow the P2–Na2/3Ni1/3Mn2/3O2 electrode with a relatively high operating voltage and high specific capacity. However, the phase transition from P2 to O2 and Na+/vacancy ordering make P2–Na2/3Ni1/3Mn2/3O2 susceptible to severe voltage and capacity decay. Herein, we propose to employ the electrochemically active copper(II) as a unique substituent to stabilize the P2 phase, forming Na0.67Ni0.3−xCuxMn0.7O2 (x = 0, 0.1, 0.2 and 0.3). Our work highlights the importance of Cu(II) in the structural engineering of high performance cathode materials, whose existence can not only stabilize the P2 phase against the notorious phase transition, but also contribute to the rechargeable capacity due to the high potential Cu2+/Cu3+ redox. We identified that the cathode formulated as P2-type Na0.67Ni0.1Cu0.2Mn0.7O2 shows favorable battery performance with much-alleviated structural degradation.

Fe3O4-functionalized graphene nanosheet embedded phase change material composites: efficient magnetic- and sunlight-driven energy conversion and storage

Abstract: As an important energy utilization mode, thermal energy is closely related to human life and social production. Phase change materials have been widely adopted to store thermal energy to improve its utilization efficiency. However, the inherent low energy conversion ability of these materials is one of the key problems to be resolved urgently. In this paper, we report novel magnetic- and sunlight-driven energy conversion and storage nanocomposites based on Fe3O4-functionalized graphene nanosheet (Fe3O4–GNS) embedded form-stable polymer phase change materials. Owing to the excellent magnetocaloric performance of Fe3O4 and the universal photoabsorption and photothermal conversion of graphene, the nanocomposites can effectively convert magnetic or light energy into thermal energy under an alternating magnetic field or solar illumination. The energy is stored by phase change materials during the phase transition process. The obtained hybrid nanocomposites exhibit excellent thermal stability with high melting–freezing enthalpy and excellent reversibility. Furthermore, the novel nanocomposites show the characteristics of form-stable phase transformation. The Fe3O4–GNS embedded phase change material composites for energy conversion and storage are expected to open up a rich field of energy materials.

High pressure synthesis of a hexagonal close-packed phase of the high-entropy alloy CrMnFeCoNi

Abstract: High-entropy alloys, near-equiatomic solid solutions of five or more elements, represent a new strategy for the design of materials with properties superior to those of conventional alloys. However, their phase space remains constrained, with transition metal high-entropy alloys exhibiting only face- or body-centered cubic structures. Here, we report the high-pressure synthesis of a hexagonal close-packed phase of the prototypical high-entropy alloy CrMnFeCoNi. This martensitic transformation begins at 14 GPa and is attributed to suppression of the local magnetic moments, destabilizing the initial fcc structure. Similar to fcc-to-hcp transformations in Al and the noble gases, the transformation is sluggish, occurring over a range of >40 GPa. However, the behaviour of CrMnFeCoNi is unique in that the hcp phase is retained following decompression to ambient pressure, yielding metastable fcc-hcp mixtures. This demonstrates a means of tuning the structures and properties of high-entropy alloys in a manner not achievable by conventional processing techniques. High-entropy alloys represent a new strategy for the design of materials with properties superior to those of conventional alloys, but are largely limited to simple phases of cubic symmetry. By applying high pressures on CrMnFeCoNi, here authors demonstrate synthesis of a hexagonal close-packed phase.

A comprehensive study on the structural evolution of HfO2 thin films doped with various dopants

Abstract: The origin of the unexpected ferroelectricity in doped HfO2 thin films is now considered to be the formation of a non-centrosymmetric Pca21 orthorhombic phase. Due to the polycrystalline nature of the films as well as their extremely small thickness (∼10 nm) and mixed orientation and phase composition, structural analysis of doped HfO2 thin films remains a challenging task. As a further complication, the structural similarities of the orthorhombic and tetragonal phase are difficult to distinguish by typical structural analysis techniques such as X-ray diffraction. To resolve this issue, the changes in the grazing incidence X-ray diffraction (GIXRD) patterns of HfO2 films doped with Si, Al, and Gd are systematically examined. For all dopants, the shift of o111/t101 diffraction peak is observed with increasing atomic layer deposition (ALD) cycle ratio, and this shift is thought to originate from the orthorhombic to P42/nmc tetragonal phase transition with decreasing aspect ratio (2a/(b + c) for orthorhombic and c/a for the tetragonal phase). For quantitative phase analysis, Rietveld refinement is applied to the GIXRD patterns. A progressive phase transition from P21/c monoclinic to orthorhombic to tetragonal is confirmed for all dopants, and a strong relationship between orthorhombic phase fraction and remanent polarization value is uniquely demonstrated. The concentration range for the ferroelectric properties was the narrowest for the Si-doped HfO2 films. The dopant size is believed to strongly affect the concentration range for the ferroelectric phase stabilization, since small dopants can strongly decrease the free energy of the tetragonal phase due to their shorter metal–oxygen bonds.

Decoding the phase structure of QCD via particle production at high energy

Abstract: Recent studies based on non-perturbative lattice Monte-Carlo solutions of Quantum Chromodynamics, the theory of strong interactions, demonstrated that at high temperature there is a phase change from confined hadronic matter to a deconfined quark-gluon plasma where quarks and gluons can travel distances largely exceeding the size of hadrons. The phase structure of such strongly interacting matter can be decoded via analysis of particle abundances in high energy nuclear collisions within the framework of the statistical hadronization approach. The results imply quark-hadron duality at and experimental delineation of the location of the phase boundary of strongly interacting matter.

The Metal–Support Interaction Concerning the Particle Size Effect of Pd/Al2O3 on Methane Combustion

Abstract: The particle size effect of Pd nanoparticles supported on alumina with various crystalline phases on methane combustion was investigated. Pd/θ, α-Al2 O3 with weak metal-support interaction showed a volcano-shaped dependence of the catalytic activity on the size of Pd particles, and the catalytic activity of the strongly interacted Pd/γ-Al2 O3 increased with the particle size. Based on a structural analysis of Pd nanoparticles using CO adsorption IR spectroscopy and spherical aberration-corrected scanning/transmission electron microscopy, the dependence of catalytic activity on Pd particle size and the alumina crystalline phase was due to the fraction of step sites on Pd particle surface. The difference in fraction of the step site is derived from the particle shape, which varies not only with Pd particle size but also with the strength of metal-support interaction. Therefore, this interaction perturbs the particle size effect of Pd/Al2 O3 for methane combustion.

Piezochromic Carbon Dots with Two-photon Fluorescence

Abstract: Piezochromic materials, which show color changes resulting from mechanical grinding or external pressure, can be used as mechanosensors, indicators of mechano-history, security papers, optoelectronic devices, and data storage systems. A class of piezochromic materials with unprecedented two-photon absorptive and yellow emissive carbon dots (CDs) was developed for the first time. Applied pressure from 0–22.84 GPa caused a noticeable color change in the luminescence of yellow emissive CDs, shifting from yellow (557 nm) to blue-green (491 nm). Moreover, first-principles calculations support transformation of the sp2 domains into sp3-hybridized domains under high pressure. The structured CDs generated were captured by quenching the high-pressure phase to ambient conditions, thus greatly increasing the choice of materials available for a variety of applications.

Probing slow relaxation and many-body localization in two-dimensional quasiperiodic systems

Abstract: While many-body localization is well understood in one-dimensional systems, its behavior in two or more dimensions is largely unknown. New experiments hint at a many-body localized phase in a two-dimensional system and provide insight into how a system transitions between this phase and a normal thermal phase.

Surface tension prevails over solute effect in organic-influenced cloud droplet activation

Abstract: The spontaneous growth of cloud condensation nuclei (CCN) into cloud droplets under supersaturated water vapour conditions is described by classic Kohler theory. This spontaneous activation of CCN depends on the interplay between the Raoult effect, whereby activation potential increases with decreasing water activity or increasing solute concentration, and the Kelvin effect, whereby activation potential decreases with decreasing droplet size or increases with decreasing surface tension, which is sensitive to surfactants. Surface tension lowering caused by organic surfactants, which diminishes the Kelvin effect, is expected to be negated by a concomitant reduction in the Raoult effect, driven by the displacement of surfactant molecules from the droplet bulk to the droplet–vapour interface. Here we present observational and theoretical evidence illustrating that, in ambient air, surface tension lowering can prevail over the reduction in the Raoult effect, leading to substantial increases in cloud droplet concentrations. We suggest that consideration of liquid–liquid phase separation, leading to complete or partial engulfing of a hygroscopic particle core by a hydrophobic organic-rich phase, can explain the lack of concomitant reduction of the Raoult effect, while maintaining substantial lowering of surface tension, even for partial surface coverage. Apart from the importance of particle size and composition in droplet activation, we show by observation and modelling that incorporation of phase-separation effects into activation thermodynamics can lead to a CCN number concentration that is up to ten times what is predicted by climate models, changing the properties of clouds. An adequate representation of the CCN activation process is essential to the prediction of clouds in climate models, and given the effect of clouds on the Earth’s energy balance, improved prediction of aerosol–cloud–climate interactions is likely to result in improved assessments of future climate change.

Self-Optimization of the Active Site of Molybdenum Disulfide by an Irreversible Phase Transition during Photocatalytic Hydrogen Evolution

Abstract: The metallic 1T-MoS2 has attracted considerable attention as an effective catalyst for hydrogen evolution reactions (HERs). However, the fundamental mechanism about the catalytic activity of 1T-MoS2 and the associated phase evolution remain elusive and controversial. Herein, we prepared the most stable 1T-MoS2 by hydrothermal exfoliation of MoS2 nanosheets vertically rooted into rigid one-dimensional TiO2 nanofibers. The 1T-MoS2 can keep highly stable over one year, presenting an ideal model system for investigating the HER catalytic activities as a function of the phase evolution. Both experimental studies and theoretical calculations suggest that 1T phase can be irreversibly transformed into a more active 1T' phase as true active sites in photocatalytic HERs, resulting in a "catalytic site self-optimization". Hydrogen atom adsorption is the major driving force for this phase transition.

Depinning and nonequilibrium dynamic phases of particle assemblies driven over random and ordered substrates: a review.

Abstract: We review the depinning and nonequilibrium phases of collectively interacting particle systems driven over random or periodic substrates. This type of system is relevant to vortices in type-II superconductors, sliding charge density waves, electron crystals, colloids, stripe and pattern forming systems, and skyrmions, and could also have connections to jamming, glassy behaviors, and active matter. These systems are also ideal for exploring the broader issues of characterizing transient and steady state nonequilibrium flow phases as well as nonequilibrium phase transitions between distinct dynamical phases, analogous to phase transitions between different equilibrium states. We discuss the differences between elastic and plastic depinning on random substrates and the different types of nonequilibrium phases which are associated with specific features in the velocity-force curves, fluctuation spectra, scaling relations, and local or global particle ordering. We describe how these quantities can change depending on the dimension, anisotropy, disorder strength, and the presence of hysteresis. Within the moving phase we discuss how there can be a transition from a liquid-like state to dynamically ordered moving crystal, smectic, or nematic states. Systems with periodic or quasiperiodic substrates can have multiple nonequilibrium second or first order transitions in the moving state between chaotic and coherent phases, and can exhibit hysteresis. We also discuss systems with competing repulsive and attractive interactions, which undergo dynamical transitions into stripes and other complex morphologies when driven over random substrates. Throughout this work we highlight open issues and future directions such as absorbing phase transitions, nonequilibrium work relations, inertia, the role of non-dissipative dynamics such as Magnus effects, and how these results could be extended to the broader issues of plasticity in crystals, amorphous solids, and jamming phenomena.

Structure of a model TiO2 photocatalytic interface

Abstract: The interaction of water with TiO2 is crucial to many of its practical applications, including photocatalytic water splitting. Following the first demonstration of this phenomenon 40 years ago there have been numerous studies of the rutile single-crystal TiO2(110) interface with water. This has provided an atomic-level understanding of the water-TiO2 interaction. However, nearly all of the previous studies of water/TiO2 interfaces involve water in the vapour phase. Here, we explore the interfacial structure between liquid water and a rutile TiO2(110) surface pre-characterized at the atomic level. Scanning tunnelling microscopy and surface X-ray diffraction are used to determine the structure, which is comprised of an ordered array of hydroxyl molecules with molecular water in the second layer. Static and dynamic density functional theory calculations suggest that a possible mechanism for formation of the hydroxyl overlayer involves the mixed adsorption of O2 and H2O on a partially defected surface. The quantitative structural properties derived here provide a basis with which to explore the atomistic properties and hence mechanisms involved in TiO2 photocatalysis.

Critical Properties of the Many-Body Localization Transition

Abstract: Some quantum systems can enter a many-body localized (MBL) phase, where the particles do not settle into thermal equilibrium but remain stuck in some initial state. A new theoretical analysis explores the transition between MBL and thermal phases and finds that the transition is driven by the growth of a network of quantum entanglement.

Coplanar semiconductor–metal circuitry defined on few-layer MoTe 2 via polymorphic heteroepitaxy

Abstract: Crystal polymorphism selectively stabilizes the electronic phase of atomically thin transition-metal dichalcogenides (TMDCs) as metallic or semiconducting, suggesting the potential to integrate these polymorphs as circuit components in two-dimensional electronic circuitry. Developing a selective and sequential growth strategy for such two-dimensional polymorphs in the vapour phase is a critical step in this endeavour. Here, we report on the polymorphic integration of distinct metallic (1T′) and semiconducting (2H) MoTe2 crystals within the same atomic planes by heteroepitaxy. The realized polymorphic coplanar contact is atomically coherent, and its barrier potential is spatially tight-confined over a length of only a few nanometres, with a lowest contact barrier height of ∼25 meV. We also demonstrate the generality of our synthetic integration approach for other TMDC polymorph films with large areas. Sequential heteroepitaxy of transition-metal dichalcogenide polymorphs with different electronic properties is used to build coplanar ultrathin circuitry with atomic-scale precision.

Understanding limiting factors in thick electrode performance as applied to high energy density Li-ion batteries

Abstract: Increasing electrode thickness, thus increasing the volume ratio of active materials, is one effective method to enable the development of high energy density Li-ion batteries. In this study, an energy density versus power density optimization of LiNi0.8Co0.15Al0.05O2 (NCA)/graphite cell stack was conducted via mathematical modeling. The energy density was found to have a maximum point versus electrode thickness (critical thickness) at given discharging C rates. The physics-based factors that limit the energy/power density of thick electrodes were found to be increased cell polarization and underutilization of active materials. The latter is affected by Li-ion diffusion in active materials and Li-ion depletion in the electrolyte phase. Based on those findings, possible approaches were derived to surmount the limiting factors. The improvement of the energy–power relationship in an 18,650 cell was used to demonstrate how to optimize the thick electrode parameters in cell engineering.