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Zhou, Lin

Publications and source records attributed to Zhou, Lin.

At least 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Unprecedented generation of 3D heterostructures by mechanochemical disassembly and re-ordering of incommensurate metal chalcogenides

Three-dimensional heterostructures are usually created either by assembling two-dimensional building blocks into hierarchical architectures or using stepwise chemical processes that sequentially deposit individual monolayers. Both approaches suffer from a number of issues, including lack of suitable precursors, limited reproducibility, and poor scalability of the preparation protocols. Therefore, development of alternative methods that enable preparation of heterostructured materials is desired. We create heterostructures with incommensurate arrangements of well-defined building blocks using a synthetic approach that comprises mechanical disassembly and simultaneous reordering of layered transition-metal dichalcogenides, MX 2 , and non-layered monochalcogenides, REX, where M = Ta, Nb, RE = Sm, La, and X = S, Se. We show that the discovered solid-state processes are rooted in stochastic mechanochemical transformations directed by electronic interaction between chemically and structurally dissimilar solids toward atomic-scale ordering, and offer an alternative to conventional heterostructuring. Details of composition–structure–properties relationships in the studied materials are also highlighted.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Single-atom-layer traps in a solid electrolyte for lithium batteries

In order to fully understand the lithium-ion transport mechanism in solid electrolytes for batteries, not only the periodic lattice but also the non-periodic features that disrupt the ideal periodicity must be comprehensively studied. At present only a limited number of non-periodic features such as point defects and grain boundaries are considered in mechanistic studies. Here, we discover an additional type of non-periodic feature that significantly influences ionic transport; this feature is termed a “single-atom-layer trap” (SALT). In a prototype solid electrolyte Li 0.33 La 0.56 TiO 3 , the single-atom-layer defects that form closed loops, i.e., SALTs, are found ubiquitous by atomic-resolution electron microscopy. According to ab initio calculations, these defect loops prevent large volumes of materials from participating in ionic transport, and thus severely degrade the total conductivity. This discovery points out the urgency of thoroughly investigating different types of non-periodic features, and motivates similar studies for other solid electrolytes.

25 ENERGY STORAGE↗
DOE OSTI2020

Mechanisms of Skyrmion and Skyrmion Crystal Formation from the Conical Phase

Real-space topological magnetic structures such as skyrmions and merons are promising candidates for information storage and transport. However, the microscopic mechanisms that control their formation and evolution are still unclear. In this work, using in situ Lorentz transmission electron microscopy, we demonstrate that skyrmion crystals (SkXs) can nucleate, grow, and evolve from the conical phase in the same ways that real nanocrystals form from vapors or solutions. More intriguingly, individual skyrmions can also “reproduce” by division in a mitosis-like process that allows them to annihilate SkX lattice imperfections, which is not available to crystals made of mass-conserving particles. Combined string method and micromagnetic calculations show that competition between repulsive and attractive interactions between skyrmions governs particle-like SkX growth, but nonconservative SkX growth appears to be defect mediated. Our results provide insights toward manipulating magnetic topological states by applying established crystal growth theory, adapted to account for the new process of skyrmion mitosis.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Identifying the Molecular Edge Termination of Exfoliated Hexagonal Boron Nitride Nanosheets with Solid-State NMR Spectroscopy and Plane-Wave DFT Calculations

Hexagonal boron nitride nanosheets (h-BNNS), the isoelectronic analog to graphene, have received interest over the past decade due to their high thermal oxidative resistance, high bandgap, catalytic activity, and low cost. The functional groups that terminate boron and nitrogen zigzag and/or armchair edges directly affect their chemical, physical, and electronic properties. However, an understanding of the molecular edge termination present in h-BNNS is lacking. Here, high-resolution magic-angle spinning (MAS) solid-state NMR (SSNMR) spectroscopy, and plane-wave density-functional theory (DFT) calculations are used to determine the molecular edge termination in exfoliated h-BNNS. 1 H → 11 B cross-polarization MAS (CPMAS) SSNMR spectra of h-BNNS revealed multiple hydroxyl/oxygen coordinated boron edge sites that were not detectable in direct excitation experiments. A dynamic nuclear polarization (DNP)-enhanced 1 H → 15 N CPMAS spectrum of h-BNNS displayed four distinct 15 N resonances while a 2D 1 H{ 14 N} dipolar-HMQC spectrum acquired with fast MAS revealed three distinct 14 N environments. Plane-wave DFT calculations were used to construct model edge structures and predict the corresponding 11 B, 14 N and 15 N SSNMR spectra. Comparison of the experimental and predicted SSNMR spectra confirms that zigzag and armchair edges with both amine and boron hydroxide/oxide termination are present. The detailed characterization of h-BNNS molecular edge termination will prove useful for many material science applications. The techniques outlined here should also be applicable to understand the molecular edge terminations in other 2D materials

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Managing hysteresis of Gd 5 Si 2 Ge 2 by magnetic field cycling

The influence of magnetic field cycling through the first-order magnetostructural transformation on the magnetic and magnetocaloric properties, as well as hysteresis of polycrystalline Gd 5 Si 2 Ge 2 , has been studied using magnetometry. Here, the cycling has a minimal effect on the magnetic field-induced entropy change and the phase transformation temperature of the material. On the other hand, magnetic hysteresis decreases by 30% after approximately ten cycles and remains low unless the sample is moved far into the paramagnetic regime. Factors playing a role in the history dependence of hysteresis have been discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Fatigue-resistant high-performance elastocaloric materials made by additive manufacturing

Elastocaloric cooling, a solid-state cooling technology, displays the latent heat released and absorbed by stress-induced phase transformations. Hysteresis associated with transformation, however, is detrimental to efficient energy conversion and functional durability. Here, we have created thermodynamically efficient, low-hysteresis elastocaloric cooling materials by means of additive manufacturing of nickel-titanium. The utilization of a localized molten environment and near-eutectic mixing of elemental powders has led to the formation of nanocomposite microstructures composed of a nickel-rich intermetallic compound interspersed among a binary alloy matrix. The microstructure allowed extremely small hysteresis in quasi-linear stress-strain behaviors—enhancing the materials efficiency by a factor of four to seven—and repeatable elastocaloric performance over 1 million cycles. Implementing additive manufacturing to elastocaloric cooling materials enables distinct microstructure control of high-performance metallic refrigerants with long fatigue life.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Integrating Rh Species with NiFe-Layered Double Hydroxide for Overall Water Splitting

NiFe-layered double hydroxide (LDH) is thought of as a promising bifunctional water-splitting catalyst, owing to its excellent performances for alkaline oxygen evolution reactions (OERs). However, it shows extremely poor activity toward hydrogen evolution reactions (HERs) due to the weak hydrogen adsorption. We demonstrated that the integration of Rh species and NiFe-LDH can dramatically improve its HER kinetics without sacrificing the OER performance. The Rh species were initially integrated into NiFe-LDH as oxidized dopants and metallic clusters (< 1 nm). In 1 M KOH electrolyte, an overpotential of 58 mV is needed to catalyze 10 mA cm –2 HER current density. Furthermore, this catalyst only requires 1.46 V to drive an electrolyzer at 10 mA cm –2 . A strong interaction between metallic Rh clusters and NiFe hydroxide during the HER process is revealed. The theoretical calculation shows the Rh ions replace Fe ions as the major active sites that are responsible for OERs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Uncompensated Polarization in Incommensurate Modulations of Perovskite Antiferroelectrics

Complex polar structures of incommensurate modulations (ICMs) are revealed in chemically modified PbZrO 3 perovskite antiferroelectrics using advanced transmission electron microscopy techniques. The Pb-cation displacements, previously assumed to arrange in a fully compensated antiparallel fashion, are found to be either antiparallel, but with different magnitudes, or in a nearly orthogonal arrangement in adjacent stripes in the ICMs. Ab initio calculations corroborate the low-energy state of these arrangements. Our discovery corrects the atomic understanding of ICMs in PbZrO 3 -based perovskite antiferroelectrics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

In-situ TEM analysis of the phase transformation mechanism of a Cu–Al–Ni shape memory alloy

We report that minimizing phase transformation (PT) hysteresis is of crucial importance for reliability of shape memory alloy (SMA)-based devices, where the lattice strain/stress caused by thermal hysteresis leads to functional degradation. As a result, understanding structural factors that control PT pathway is critical for development of materials with high reversibility. In this study, two distinct PT mechanisms (from γ$'\atop{1}$ martensite to β 1 austenite phase) in Cu–Al–Ni SMAs were revealed by in-situ TEM observation. A growth-dominant conventional PT mechanism shows in the fast quench sample, whereas a nucleation-dominant PT mechanism that suppresses interface propagation and induces high thermal hysteresis displays in the slow quench sample. By characterizing the atomic scale composition and microstructure we discover that slow quenching induces nanoprecipitation that changes chemistry of the matrix alloy, which in turn causes the higher PT hysteresis and temperature, while fast quenching avoids the formation of these nanoprecipitates. Lastly, our finding provides valuable insights into the fabrication of SMAs with better reliability.

36 MATERIALS SCIENCE↗
DOE OSTI2019

In situ TEM study of the transitions between crystalline Si and nonstoichiometric amorphous oxide under bipolar voltage bias

The electrical responses, either structurally or chemically, at the interface between a SiO 2 thin film and a single crystalline Si substrate are an important research subject in Si-based devices. Dielectric breakdown-induced epitaxial migration of Si into SiO 2 has been reported as a degradation mechanism in field effect transistors (FETs). Here, we show a direct observation of electric field induced conversion of single crystalline Si to nonstoichiometric amorphous oxide starting from the Si/native oxide interface using in situ transmission electron microscopy (TEM). We further show that nanocrystalline Si can form in the amorphous oxide under a voltage bias of reversed polarity. Electron energy loss spectroscopy and energy dispersive X-ray spectroscopy analyses indicate that the observed amorphization process was caused by the oxidation of Si and the recrystallization process was caused by the reduction of nonstoichiometric amorphous silicon oxide. Furthermore, both transitions are a result of field-driven directional migration of oxygen which originally comes from its native oxide layer.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Investigation of Powder Processing, Heat Treating, and Texturing to Improve Gas Atomized alnico Magnets for use in Electric Drive Motors

Alnico permanent magnet materials have been proposed as a rare earth free permanent magnet alternative during an ongoing search to replace rare earth permanent magnets that are used for interior permanent magnet motors, a common motor found in electric vehicles. A powder processing approach was used to study two alnico alloys (Full-Co and lower cost Co-Lean, both with enhanced coercivity) to anticipate high volume manufacturing needed to supply millions of permanent magnets to interior permanent magnet motors. In this study the two alloys were gas atomized, compression molded, and solid-state sintered to fabricate near-final shape alnico magnets. The Full-Co displayed abnormal grain growth (resulting in >1 mm size grains) during sintering while the Co-Lean did not (~20 μm – 400 μm sized grains depending on the sintering hold times). Solid state grain alignment was used to promote a <001> textured (easy axis) microstructure to enhance magnetic properties, yet both alloys did not show predicted grain alignment behavior. Comparisons of the powder processing, microstructures, and magnetic properties of the two alloys will be discussed, as well as an evaluation as to why non-theoretical processing behavior of the Full-Co and Co-Lean alnico permanent magnets is occurring. Preliminary interior permanent magnet motor designs for alnico magnets are discussed, as this is the overarching objective for powder-based alnico permanent magnets.

Rinko, Emily↗