Organic–inorganic lead halide perovskites(LHPs) have attracted great interest owing to their outstanding optoelectronic properties.Typically,the underlying electronic structure would determinate the physical properti...Organic–inorganic lead halide perovskites(LHPs) have attracted great interest owing to their outstanding optoelectronic properties.Typically,the underlying electronic structure would determinate the physical properties of materials.But as for now,limited studies have been done to reveal the underlying electronic structure of this material system,comparing to the huge amount of investigations on the material synthesis.The effective mass of the valance band is one of the most important physical parameters which plays a dominant role in charge transport and photovoltaic phenomena.In pristine CsPbBr_(3),the Fr?hlich polarons associated with the Pb–Br stretching modes are proposed to be responsible for the effective mass renormalization.In this regard,it would be very interesting to explore the electronic structure in doped LHPs.Here,we report high-resolution angle-resolved photoemission spectroscopy(ARPES) studies on both pristine and Cl-doped CsPbBr_(3).The experimental band dispersions are extracted from ARPES spectra along both ■ and ■ high symmetry directions.DFT calculations are performed and directly compared with the ARPES data.Our results have revealed the band structure of Cl-doped CsPbBr_(3) for the first time,which have also unveiled the effective mass renormalization in the Cl-doped CsPbBr_(3) compound.Doping dependent measurements indicate that the chlorine doping could moderately tune the renormalization strength.These results will help understand the physical properties of LHPs as a function of doping.展开更多
Understanding the behavior of matter at extreme pressures of the order of a megabar(Mbar)is essential to gain insight into various physical phenomena at macroscales—the formation of planets,young stars,and the cores ...Understanding the behavior of matter at extreme pressures of the order of a megabar(Mbar)is essential to gain insight into various physical phenomena at macroscales—the formation of planets,young stars,and the cores of super-Earths,and at microscales—damage to ceramic materials and high-pressure plastic transformation and phase transitions in solids.Under dynamic compression of solids up to Mbar pressures,even a solid with high strength exhibits plastic properties,causing the induced shock wave to split in two:an elastic precursor and a plastic shock wave.This phenomenon is described by theoretical models based on indirect measurements of material response.The advent of x-ray free-electron lasers(XFELs)has made it possible to use their ultrashort pulses for direct observations of the propagation of shock waves in solid materials by the method of phase-contrast radiography.However,there is still a lack of comprehensive data for verification of theoretical models of different solids.Here,we present the results of an experiment in which the evolution of the coupled elastic-plastic wave structure in diamond was directly observed and studied with submicrometer spatial resolution,using the unique capabilities of the x-ray free-electron laser(XFEL).The direct measurements allowed,for the first time,the fitting and validation of the 2D failure model for diamond in the range of several Mbar.Our experimental approach opens new possibilities for the direct verification and construction of equations of state of matter in the ultra-high-stress range,which are relevant to solving a variety of problems in high-energy-density physics.展开更多
Compelling evidence indicates that the solid Earth consists of two physicochemically distinct zones separated radially in the middle of the lower mantle at∼1800 km depth.The inner zone is governed by pressure-induced...Compelling evidence indicates that the solid Earth consists of two physicochemically distinct zones separated radially in the middle of the lower mantle at∼1800 km depth.The inner zone is governed by pressure-induced physics and chemistry dramatically different from the conventional behavior in the outer zone.These differences generate large physical and chemical potentials between the two zones that provide fundamental driving forces for triggering major events in Earth’s history.One of the main chemical carriers between the two zones isH_(2)Oin hydrous minerals that subducts into the inner zone,releases hydrogen,and leaves oxygen to create superoxides and form oxygen-rich piles at the core–mantle boundary,resulting in localized net oxygen gain in the inner zone.Accumulation of oxygen-rich piles at the base of the mantle could eventually reach a supercritical level that triggers eruptions,injecting materials that cause chemical mantle convection,superplumes,large igneous provinces,extreme climate changes,atmospheric oxygen fluctuations,and mass extinctions.Interdisciplinary research will be the key for advancing a unified theory of the four-dimensional Earth system.展开更多
Carbon materials have been playing important roles in advancing energyrelated technologies and offering great promise to addressing the rising global energy demands and environmental issues.Nanodiamonds,an exciting cl...Carbon materials have been playing important roles in advancing energyrelated technologies and offering great promise to addressing the rising global energy demands and environmental issues.Nanodiamonds,an exciting class of carbon materials,with excellent mechanical,chemical,electronic,and optical properties,have great potentials in energy-related applications.In this contribution,we summarized some of the recent progress on nanodiamonds for energy storage,conversion,and other related applications in sustainable energy research.We discussed the promising opportunities and outlooks for nanodiamonds in energy-related fields.展开更多
Coupling nanoscale transmission X-ray microscopy (nanoTXM) with a diamond anvil cell (DAC) has exciting potential as a powerful three-dimensional probe for non-destructive imaging at high spatial resolution of materia...Coupling nanoscale transmission X-ray microscopy (nanoTXM) with a diamond anvil cell (DAC) has exciting potential as a powerful three-dimensional probe for non-destructive imaging at high spatial resolution of materials under extreme conditions. In this article, we discuss current developments in high-resolution X-ray imaging and its application in high-pressure nanoTXM experiments in a DAC with third-generation synchrotron X-ray sources, including technical considerations for preparing successful measurements. We then present results from a number of recent in situ high-pressure measurements investigating equations of state (EOS) in amorphous or poorly crystalline materials and in pressureinduced phase transitions and electronic changes. These results illustrate the potential this technique holds for addressing a wide range of research areas, ranging from condensed matter physics and solidstate chemistry to materials science and planetary interiors. Future directions for this exciting technique and opportunities to improve its capabilities for broader application in high-pressure science are discussed.展开更多
Ni-Ti-based shape memory alloys(SMAs)have found widespread use in the last 70 years,but improving their functional stability remains a key quest for more robust and advanced applications.Named for their ability to ret...Ni-Ti-based shape memory alloys(SMAs)have found widespread use in the last 70 years,but improving their functional stability remains a key quest for more robust and advanced applications.Named for their ability to retain their processed shape as a result of a reversible martensitic transformation,SMAs are highly sensitive to compositional variations.Alloying with ternary and quaternary elements to finetune the lattice parameters and the thermal hysteresis of an SMA,therefore,becomes a challenge in materials exploration.Combinatorial materials science allows streamlining of the synthesis process and data management from multiple characterization techniques.In this study,a composition spread of Ni-Ti-Cu-V thin-film library was synthesized by magnetron co-sputtering on a thermally oxidized Si wafer.Composition-dependent phase transformation temperature and microstructure were investigated and determined using high-throughput wavelength dispersive spectroscopy,synchrotron X-ray diffraction,and temperature-dependent resistance measurements.Of the 177 compositions in the materials library,32 were observed to have shape memory effect,of which five had zero or near-zero thermal hysteresis.These compositions provide flexibility in the operating temperature regimes that they can be used in.A phase map for the quaternary system and correlations of functional properties are discussed w让h respect to the local microstructure and composition of the thin-film library.展开更多
The well-known anti-corrosive property of stainless steels is largely attributed to the addition of Cr,which can assist in forming an inert film on the corroding surface.To maximize the corrosion-resistant ability of ...The well-known anti-corrosive property of stainless steels is largely attributed to the addition of Cr,which can assist in forming an inert film on the corroding surface.To maximize the corrosion-resistant ability of Cr,a thorough study dealing with the passivation behaviors of this metal,including the structure and composition of the passive film as well as related reaction mechanisms,is required.Here,continuous electrochemical adsorptions of OH-groups of water molecules onto Cr terraces in acid solutions are investigated using DFT methods.Different models with various surface conditions are applied.Passivation is found to begin in the active region,and a fully coated surface mainly with oxide is likely to be the starting point of the passive region.The calculated limiting potentials are in reasonable agreement with passivation potentials observed via experiment.展开更多
Personal thermal management is emerging as a promising strategy to provide thermal comfort for the human body while conserving energy.By improving control over the heat dissipating from the human body,personal thermal...Personal thermal management is emerging as a promising strategy to provide thermal comfort for the human body while conserving energy.By improving control over the heat dissipating from the human body,personal thermal management can provide effective personal cooling and warming.Here,we propose a facile surface modification approach to tailor the thermal conduction and radiation properties based on commercially available fabrics,to realize better management of the whole heat transport pathway from the human body to the ambient.A bifunctional asymmetric fabric(BAF)offering both a cooling and a warming effect is demonstrated.Due to the advantages of roughness asymmetry and surface modification,the BAF demonstrates an effective cooling effect through enhanced heat conduction and radiation in the cooling mode;in the warming mode,heat dissipation along both routes is reduced for personal warming.As a result,a 4.6℃ skin temperature difference is measured between the cooling and warming BAF modes,indicating that the thermal comfort zone of the human body can be enlarged with one piece of BAF clothing.We expect this work to present new insights for the design of personal thermal management textiles as well as a novel solution for the facile modification of available fabrics for both personal cooling and warming.展开更多
Diamond anvil cell techniques have been improved to allow access to the multimegabar ultrahigh-pressure region for exploring novel phenomena in condensedmatter.However,the onlyway to determine crystal structures of ma...Diamond anvil cell techniques have been improved to allow access to the multimegabar ultrahigh-pressure region for exploring novel phenomena in condensedmatter.However,the onlyway to determine crystal structures of materials above 100 GPa,namely,X-ray diffraction(XRD),especially for lowZ materials,remains nontrivial in the ultrahigh-pressure region,even with the availability of brilliant synchrotron X-ray sources.In thiswork,we performa systematic study,choosing hydrogen(the lowest X-ray scatterer)as the subject,to understand how to better perform XRD measurements of low Z materials at multimegabar pressures.The techniques that we have developed have been proved to be effective in measuring the crystal structure of solid hydrogen up to 254GPa at room temperature[C.Ji et al.,Nature 573,558–562(2019)].Wepresent our discoveries and experienceswith regard to several aspects of thiswork,namely,diamond anvil selection,sample configuration for ultrahigh-pressure XRDstudies,XRDdiagnostics for low Z materials,and related issues in data interpretation and pressure calibration.Webelieve that these methods can be readily extended to other low Z materials and can pave the way for studying the crystal structure of hydrogen at higher pressures,eventually testing structural models of metallic hydrogen.展开更多
P2-type sodium layered oxide cathode (Na_(2/3)Ni_(1/3)Mn_(2/3)O_(2)P2-NNMO) has attracted great attention as a promising cathode material for sodium ion batteries because of its high specific capacity. However, this m...P2-type sodium layered oxide cathode (Na_(2/3)Ni_(1/3)Mn_(2/3)O_(2)P2-NNMO) has attracted great attention as a promising cathode material for sodium ion batteries because of its high specific capacity. However, this material suffers from a rapid capacity fade during high-voltage cycling. Several mechanisms have been proposed to explain the capacity fade, including intragranular fracture caused by the P2-O2 phase transion, surface structural change, and irreversible lattice oxygen release. Here we systematically investigated the morphological, structural, and chemical changes of P2-NNMO during high-voltage cycling using a variety of characterization techniques. It was found that the lattice distortion and crystal-plane buckling induced by the P2-O2 phase transition slowed down the Na-ion transport in the bulk and hindered the extraction of the Na ions. The sluggish kinetics was the main reason in reducing the accessible capacity while other interfacial degradation mechanisms played minor roles. Our results not only enabled a more complete understanding of the capacity-fading mechanism of P2-NNMO but also revealed the underlying correlations between lattice doping and the moderately improved cycle performance.展开更多
The electrical conductivity of water under extreme temperatures and densities plays a central role in modeling planetary magnetic fields.Experimental data are vital to test theories of high-energy-densitywater and ass...The electrical conductivity of water under extreme temperatures and densities plays a central role in modeling planetary magnetic fields.Experimental data are vital to test theories of high-energy-densitywater and assess the possible development and presence of extraterrestrial life.These states are also important in biology and chemistry studies when specimens in water are confined and excited using ultrafast optical or free-electron lasers(FELs).Here we utilize femtosecond optical lasers to measure the transient reflection and transmission of ultrathin water sheet samples uniformly heated by a 13.6 nm FEL approaching a highly conducting state at electron temperatures exceeding 20000 K.The experiment probes the trajectory ofwater through the high-energy-density phase space and provides insights into changes in the index of refraction,charge carrier densities,andACelectrical conductivity at optical frequencies.At excitation energy densities exceeding 10MJ/kg,the index of refraction falls to n0.7,and the thermally excited free-carrier density reaches ne531027 m−3,which is over an order of magnitude higher than that of the electron carriers produced by direct photoionization.Significant specular reflection is observed owing to critical electron density shielding of electromagnetic waves.Themeasured optical conductivity reaches 23104 S/m,a value that is one to two orders of magnitude lower than those of simplemetals in a liquid state.At electron temperatures below 15000 K,the experimental results agreewell with the theoretical calculations using density-functional theory/molecular-dynamics simulations.With increasing temperature,the electron density increases and the system approaches a Fermi distribution.In this regime,the conductivities agree better with predictions from the Ziman theory of liquid metals.展开更多
A quantum spin liquid (QSL) is an exotic quantum ground state that does not break conventional symmetries and where the spins in the system remain dynamic down to zero temperature. Unlike a trivial paramagnetic state,...A quantum spin liquid (QSL) is an exotic quantum ground state that does not break conventional symmetries and where the spins in the system remain dynamic down to zero temperature. Unlike a trivial paramagnetic state, it features long-range quantum entanglement and supports fractionalized excitations.展开更多
The hierarchical structure of the composite cathodes brings in significant chemical complexity related to the interfaces,such as cathode electrolyte interphase.These interfaces account for only a small fraction of the...The hierarchical structure of the composite cathodes brings in significant chemical complexity related to the interfaces,such as cathode electrolyte interphase.These interfaces account for only a small fraction of the volume and mass,they could,however,have profound impacts on the cell-level electrochemistry.As the investigation of these interfaces becomes a crucial topic in the battery research,there is a need to properly study the surface chemistry,particularly to eliminate the biased,incomplete characterization provided by techniques that assume the homogeneous surface chemistry.Herein,we utilize nano-resolution spatially-resolved x-ray spectroscopic tools to probe the heterogeneity of the surface chemistry on LiNi0.8Mn0.1Co0.1O2 layered cathode secondary particles.Informed by the nano-resolution mapping of the Ni valance state,which serves as a measurement of the local surface chemistry,we construct a conceptual model to elucidate the electrochemical consequence of the inhomogeneous local impedance over the particle surface.Going beyond the implication in battery science,our work highlights a balance between the high-resolution probing the local chemistry and the statistical representativeness,which is particularly vital in the study of the highly complex material systems.展开更多
In this work,a one-pot strategy is presented to directly synthesize amorphous Fe_(x)Ni_(y) hydroxide nanoclusters(denoted as ANC-Fe_(x)Ni_(y),<2 nm)with oxygen vacancies induced by ionic liquids.The ANC-Fe_(x)Ni_(y...In this work,a one-pot strategy is presented to directly synthesize amorphous Fe_(x)Ni_(y) hydroxide nanoclusters(denoted as ANC-Fe_(x)Ni_(y),<2 nm)with oxygen vacancies induced by ionic liquids.The ANC-Fe_(x)Ni_(y) catalyst presents abundant catalytic sites and high intrinsic conductivity.As such,the optimized ANC-Fe_(1)Ni_(2) exhibits high activity in oxygen evolution reaction(OER)with a Tafel slope of 39 m V dec^(–1) and an overpotential of 266 m V at 10 m A cm^(-2).Notably,the optimized ANC-Fe_(1)Ni_(2) shows an extraordinarily large mass activity of 3028 Ag_(FeNi)^(–1) at the overpotential of 300 m V,which is~24-fold of commercial RuO_(2) catalyst.The superior activity of these Fe_(x)Ni_(y) hydroxide nanoclusters is ascribed to(i)the amorphous and distorted structure with abundant oxygen vacancies,and(ii)enhanced active site density by downsizing the ANC-FexNiyclusters.This strategy provides a novel route for enhancing OER electrocatalytic performance and highly encouraging for the future application of amorphous metal hydroxides in catalysis.展开更多
An experimental and simulation study of warm dense carbon foams at ambient density(ne∼10^(21) cm^(−3))is presented.This study of isochorically heated foams is motivated by their potential application in carbon-atmosp...An experimental and simulation study of warm dense carbon foams at ambient density(ne∼10^(21) cm^(−3))is presented.This study of isochorically heated foams is motivated by their potential application in carbon-atmosphere white-dwarf envelopes,where there are modeling uncertainties due to the equation of state.The foams are heated on an approximately picosecond time scale with a laser-accelerated proton beam.The cooling and expansion of the heated foams can be modeled with appropriately initialized radiation-hydrodynamics codes;xRAGE code is used in this work.The primary experimental diagnostic is the streaked optical pyrometer,which images a narrow band of radiation from the rear surface of the heated material.Presented are xRAGE modeling results for both solid aluminum targets and carbonized resorcinol-formaldehyde foam targets,showing that the foam appears to cool slowly on the pyrometer because of partial transparency.So that simulations of cooling foam are processed properly,it is necessary to account for finite optical depth in the photosphere calculation,and the methods for performing that calculation are presented in depth.展开更多
Who/what inspires you to the field of energy and nanomaterials?My Ph.D advisor Professor Charles Lieber has been a big inspiration to me since my graduate school study.I was later influenced quite a bit by my postdoct...Who/what inspires you to the field of energy and nanomaterials?My Ph.D advisor Professor Charles Lieber has been a big inspiration to me since my graduate school study.I was later influenced quite a bit by my postdoctoral mentor Professor Paul Alivisatos.By the end of my postdoctoral study in 2005,I was also influenced by Professor Steven Chu,who is a major figure to excite me to go into the energy area.I have many on‐going collaborations with Professor Chu.展开更多
Recently, the quasi-two-dimensional electron gas (q2DEG) confined at the interface between LaAlO3 and SrTiO3 has attracted significant attention. In this paper, we briefly review experimental methods that have been ...Recently, the quasi-two-dimensional electron gas (q2DEG) confined at the interface between LaAlO3 and SrTiO3 has attracted significant attention. In this paper, we briefly review experimental methods that have been used to tune the carrier density and mobility of this q2DEG. These methods can be classified into two categories: growth-related tuning (i.e. substrate, growth temperature, oxygen pressure, post-annealing, LaAlO3 thickness, stoichiometry, and capping layers) and post-growth tuning (i.e. electrostatic field gating, conductive atomic force microscopy and surface adsorbates). Taken together, these methods enable the broad tuning of the electronic properties of this interface.展开更多
Owing to their ultra-high accelerating gradients,combined with injection inside micrometer-scale accelerating wakefield buckets,plasma-based accelerators hold great potential to drive a new generation of free-electron...Owing to their ultra-high accelerating gradients,combined with injection inside micrometer-scale accelerating wakefield buckets,plasma-based accelerators hold great potential to drive a new generation of free-electron lasers(FELs).Indeed,the first demonstration of plasma-driven FEL gain was reported recently,representing a major milestone for the field.Several groups around the world are pursuing these novel light sources,with methodology varying in the use of wakefield driver(laser-driven or beam-driven),plasma structure,phase-space manipulation,beamline design,and undulator technology,among others.This paper presents our best attempt to provide a comprehensive overview of the global community efforts towards plasma-based FEL research and development.展开更多
To be useful for most scientific and medical applications,compact particle accelerators will require much higher average current than enabled by current architectures.For this purpose,we propose a photonic crystal arc...To be useful for most scientific and medical applications,compact particle accelerators will require much higher average current than enabled by current architectures.For this purpose,we propose a photonic crystal architecture for a dielectric laser accelerator,referred to as a multi-input multi-output silicon accelerator(MIMOSA),that enables simultancous acceleration of multiple electron beams,increasing the total electron throughput by at least I order of magnitude.To achieve this,we show that the photonic crystal must support a mode at the I point in reciprocal space,with a normalized frequency equal to the normalized speed of the phase-matched electron.We show that the figure of merit of the MIMOSA can be inferred from the eigenmodes of the corresponding infinitely periodic structure,which provides a powerful approach to design such devices.Additionally,we extend the MIMOSA architecture to electron deflectors and other clectron manipulation functionalities.These additional functionalities,combined with the increased electron throughput of these devices,permit all-optical on-chip manipulation of electron beams in a fully integrated architecture compatible with current fabrication technologies,which opens the way to unconventional electron beam shaping,imaging,and radiationg encration.展开更多
基金Project supported by the International Partnership Program of the Chinese Academy of Sciences(Grant No.123GJHZ2022035MI)the Fundamental Research Funds for the Central Universities(Grant Nos.WK3510000015 and WK3510000012)。
文摘Organic–inorganic lead halide perovskites(LHPs) have attracted great interest owing to their outstanding optoelectronic properties.Typically,the underlying electronic structure would determinate the physical properties of materials.But as for now,limited studies have been done to reveal the underlying electronic structure of this material system,comparing to the huge amount of investigations on the material synthesis.The effective mass of the valance band is one of the most important physical parameters which plays a dominant role in charge transport and photovoltaic phenomena.In pristine CsPbBr_(3),the Fr?hlich polarons associated with the Pb–Br stretching modes are proposed to be responsible for the effective mass renormalization.In this regard,it would be very interesting to explore the electronic structure in doped LHPs.Here,we report high-resolution angle-resolved photoemission spectroscopy(ARPES) studies on both pristine and Cl-doped CsPbBr_(3).The experimental band dispersions are extracted from ARPES spectra along both ■ and ■ high symmetry directions.DFT calculations are performed and directly compared with the ARPES data.Our results have revealed the band structure of Cl-doped CsPbBr_(3) for the first time,which have also unveiled the effective mass renormalization in the Cl-doped CsPbBr_(3) compound.Doping dependent measurements indicate that the chlorine doping could moderately tune the renormalization strength.These results will help understand the physical properties of LHPs as a function of doping.
基金We thank the technical staff of SACLA for their support during the experiment.The experiment was performed at BL3 of SACLA with the approval of the Japan Synchrotron Radiation Research Institute(Proposal Nos.2021A8004 and 2021B8002).The high-power drive laser installed in SACLA EH5 was developed with the cooperation of Hamamatsu Photonics.The installation of diffractive optical elements to improve the smoothness of the drive laser-pattern was supported by the SACLA Basic Development ProgramThe work was carried out with the financial support of the Russian Federation represented by the Ministry of Science and Higher Education of the Russian Federation(Grant No.075-15-2021-1352)This work was supported by KAKENHI(Grant Nos.17K05729 and 21K03499)from the Japan Society for the Promotion of Science(JSPS).
文摘Understanding the behavior of matter at extreme pressures of the order of a megabar(Mbar)is essential to gain insight into various physical phenomena at macroscales—the formation of planets,young stars,and the cores of super-Earths,and at microscales—damage to ceramic materials and high-pressure plastic transformation and phase transitions in solids.Under dynamic compression of solids up to Mbar pressures,even a solid with high strength exhibits plastic properties,causing the induced shock wave to split in two:an elastic precursor and a plastic shock wave.This phenomenon is described by theoretical models based on indirect measurements of material response.The advent of x-ray free-electron lasers(XFELs)has made it possible to use their ultrashort pulses for direct observations of the propagation of shock waves in solid materials by the method of phase-contrast radiography.However,there is still a lack of comprehensive data for verification of theoretical models of different solids.Here,we present the results of an experiment in which the evolution of the coupled elastic-plastic wave structure in diamond was directly observed and studied with submicrometer spatial resolution,using the unique capabilities of the x-ray free-electron laser(XFEL).The direct measurements allowed,for the first time,the fitting and validation of the 2D failure model for diamond in the range of several Mbar.Our experimental approach opens new possibilities for the direct verification and construction of equations of state of matter in the ultra-high-stress range,which are relevant to solving a variety of problems in high-energy-density physics.
基金We thank Yu He,Qingyang Hu,Jin Liu,Duckyoung Kim,and Li Zhang for sharing preliminary information.W.L.Mao acknowledges support from NSF Geophysics Grant No.EAR 1446969H.-k.Mao acknowledges supports from NSF Geochemistry Grant No.EAR-1447438+1 种基金NSF Geophysics Grant No.EAR-1722515This work was also partially supported by the National Natural Science Foundation of China Grant No.U1530402 and U1930401.
文摘Compelling evidence indicates that the solid Earth consists of two physicochemically distinct zones separated radially in the middle of the lower mantle at∼1800 km depth.The inner zone is governed by pressure-induced physics and chemistry dramatically different from the conventional behavior in the outer zone.These differences generate large physical and chemical potentials between the two zones that provide fundamental driving forces for triggering major events in Earth’s history.One of the main chemical carriers between the two zones isH_(2)Oin hydrous minerals that subducts into the inner zone,releases hydrogen,and leaves oxygen to create superoxides and form oxygen-rich piles at the core–mantle boundary,resulting in localized net oxygen gain in the inner zone.Accumulation of oxygen-rich piles at the base of the mantle could eventually reach a supercritical level that triggers eruptions,injecting materials that cause chemical mantle convection,superplumes,large igneous provinces,extreme climate changes,atmospheric oxygen fluctuations,and mass extinctions.Interdisciplinary research will be the key for advancing a unified theory of the four-dimensional Earth system.
基金We acknowledge the support from the Department of Energy,Office of Basic Energy Sciences,Division of Materials Sciences and Engineering,under contract DE‐AC02-76SF00515.
文摘Carbon materials have been playing important roles in advancing energyrelated technologies and offering great promise to addressing the rising global energy demands and environmental issues.Nanodiamonds,an exciting class of carbon materials,with excellent mechanical,chemical,electronic,and optical properties,have great potentials in energy-related applications.In this contribution,we summarized some of the recent progress on nanodiamonds for energy storage,conversion,and other related applications in sustainable energy research.We discussed the promising opportunities and outlooks for nanodiamonds in energy-related fields.
基金supported by the Department of Energy(DOE)through the Stanford Institute for Materials&Energy Sciences(DE-AC02-76SF00515)
文摘Coupling nanoscale transmission X-ray microscopy (nanoTXM) with a diamond anvil cell (DAC) has exciting potential as a powerful three-dimensional probe for non-destructive imaging at high spatial resolution of materials under extreme conditions. In this article, we discuss current developments in high-resolution X-ray imaging and its application in high-pressure nanoTXM experiments in a DAC with third-generation synchrotron X-ray sources, including technical considerations for preparing successful measurements. We then present results from a number of recent in situ high-pressure measurements investigating equations of state (EOS) in amorphous or poorly crystalline materials and in pressureinduced phase transitions and electronic changes. These results illustrate the potential this technique holds for addressing a wide range of research areas, ranging from condensed matter physics and solidstate chemistry to materials science and planetary interiors. Future directions for this exciting technique and opportunities to improve its capabilities for broader application in high-pressure science are discussed.
基金The author thanks Tieren Gao,Peer Decker,Alan Savan,and Manfred Wuttig for fruitful discussions.The authors gratefully acknowledge funding support by the National Science Foundation Graduate Research Fellowship Program(DGE 1322106).
文摘Ni-Ti-based shape memory alloys(SMAs)have found widespread use in the last 70 years,but improving their functional stability remains a key quest for more robust and advanced applications.Named for their ability to retain their processed shape as a result of a reversible martensitic transformation,SMAs are highly sensitive to compositional variations.Alloying with ternary and quaternary elements to finetune the lattice parameters and the thermal hysteresis of an SMA,therefore,becomes a challenge in materials exploration.Combinatorial materials science allows streamlining of the synthesis process and data management from multiple characterization techniques.In this study,a composition spread of Ni-Ti-Cu-V thin-film library was synthesized by magnetron co-sputtering on a thermally oxidized Si wafer.Composition-dependent phase transformation temperature and microstructure were investigated and determined using high-throughput wavelength dispersive spectroscopy,synchrotron X-ray diffraction,and temperature-dependent resistance measurements.Of the 177 compositions in the materials library,32 were observed to have shape memory effect,of which five had zero or near-zero thermal hysteresis.These compositions provide flexibility in the operating temperature regimes that they can be used in.A phase map for the quaternary system and correlations of functional properties are discussed w让h respect to the local microstructure and composition of the thin-film library.
基金financially supported by the National Key Research and Development Program of China(No.2017YFB0702100)the National Natural Science Foundation of China(Nos.51571028,51431004,and U1706221)financial support from China Scholarship Council
文摘The well-known anti-corrosive property of stainless steels is largely attributed to the addition of Cr,which can assist in forming an inert film on the corroding surface.To maximize the corrosion-resistant ability of Cr,a thorough study dealing with the passivation behaviors of this metal,including the structure and composition of the passive film as well as related reaction mechanisms,is required.Here,continuous electrochemical adsorptions of OH-groups of water molecules onto Cr terraces in acid solutions are investigated using DFT methods.Different models with various surface conditions are applied.Passivation is found to begin in the active region,and a fully coated surface mainly with oxide is likely to be the starting point of the passive region.The calculated limiting potentials are in reasonable agreement with passivation potentials observed via experiment.
文摘Personal thermal management is emerging as a promising strategy to provide thermal comfort for the human body while conserving energy.By improving control over the heat dissipating from the human body,personal thermal management can provide effective personal cooling and warming.Here,we propose a facile surface modification approach to tailor the thermal conduction and radiation properties based on commercially available fabrics,to realize better management of the whole heat transport pathway from the human body to the ambient.A bifunctional asymmetric fabric(BAF)offering both a cooling and a warming effect is demonstrated.Due to the advantages of roughness asymmetry and surface modification,the BAF demonstrates an effective cooling effect through enhanced heat conduction and radiation in the cooling mode;in the warming mode,heat dissipation along both routes is reduced for personal warming.As a result,a 4.6℃ skin temperature difference is measured between the cooling and warming BAF modes,indicating that the thermal comfort zone of the human body can be enlarged with one piece of BAF clothing.We expect this work to present new insights for the design of personal thermal management textiles as well as a novel solution for the facile modification of available fabrics for both personal cooling and warming.
基金This research was supported by the National Natural Science Foundation of China under Award No.U1930401the Department of Energy(DOE),Office of Basic Energy Science,Division of Materials Sciences and Engineering under Award No.DE-FG02-99ER45775
文摘Diamond anvil cell techniques have been improved to allow access to the multimegabar ultrahigh-pressure region for exploring novel phenomena in condensedmatter.However,the onlyway to determine crystal structures of materials above 100 GPa,namely,X-ray diffraction(XRD),especially for lowZ materials,remains nontrivial in the ultrahigh-pressure region,even with the availability of brilliant synchrotron X-ray sources.In thiswork,we performa systematic study,choosing hydrogen(the lowest X-ray scatterer)as the subject,to understand how to better perform XRD measurements of low Z materials at multimegabar pressures.The techniques that we have developed have been proved to be effective in measuring the crystal structure of solid hydrogen up to 254GPa at room temperature[C.Ji et al.,Nature 573,558–562(2019)].Wepresent our discoveries and experienceswith regard to several aspects of thiswork,namely,diamond anvil selection,sample configuration for ultrahigh-pressure XRDstudies,XRDdiagnostics for low Z materials,and related issues in data interpretation and pressure calibration.Webelieve that these methods can be readily extended to other low Z materials and can pave the way for studying the crystal structure of hydrogen at higher pressures,eventually testing structural models of metallic hydrogen.
基金financial support from the National Natural Science Foundation of China (21938005, 21573147, 22005190, 22008154, 21872163)the Science & Technology Commission of Shanghai Municipality, the Natural Science Foundation of Shanghai (19DZ1205500, 19ZR1424600, 19ZR1475100)the Sichuan Science and Technology Program (2021JDRC0015 to L.S.L)。
文摘P2-type sodium layered oxide cathode (Na_(2/3)Ni_(1/3)Mn_(2/3)O_(2)P2-NNMO) has attracted great attention as a promising cathode material for sodium ion batteries because of its high specific capacity. However, this material suffers from a rapid capacity fade during high-voltage cycling. Several mechanisms have been proposed to explain the capacity fade, including intragranular fracture caused by the P2-O2 phase transion, surface structural change, and irreversible lattice oxygen release. Here we systematically investigated the morphological, structural, and chemical changes of P2-NNMO during high-voltage cycling using a variety of characterization techniques. It was found that the lattice distortion and crystal-plane buckling induced by the P2-O2 phase transition slowed down the Na-ion transport in the bulk and hindered the extraction of the Na ions. The sluggish kinetics was the main reason in reducing the accessible capacity while other interfacial degradation mechanisms played minor roles. Our results not only enabled a more complete understanding of the capacity-fading mechanism of P2-NNMO but also revealed the underlying correlations between lattice doping and the moderately improved cycle performance.
基金supported by the U.S.Department of Energy,Office of Science,Fusion Energy Science under Grant No.FWP 100182support from the Natural Sciences and Engineering Research Council of Canada(NSERC)+4 种基金supported by the U.S.Department of Energy,Office of Science,Office of Basic Energy Sciences under Contract No.DE-AC02-76SF00515support from the U.S.Department of Energy,Laboratory Directed Research and Development(LDRD)Program at SLAC National Accelerator Laboratory,under Contract No.DE-AC02-76SF00515support within the Research Unit Grant No.FOR 2440supported in part by the U.S.Department of Energy,Office of Science,Office of Workforce Development for Teachers and Scientists(WDTS)under the Science Undergraduate Laboratory Internships(SULI)Programsupport from the LOEWE Excellence Initiative of the State of Hessen.
文摘The electrical conductivity of water under extreme temperatures and densities plays a central role in modeling planetary magnetic fields.Experimental data are vital to test theories of high-energy-densitywater and assess the possible development and presence of extraterrestrial life.These states are also important in biology and chemistry studies when specimens in water are confined and excited using ultrafast optical or free-electron lasers(FELs).Here we utilize femtosecond optical lasers to measure the transient reflection and transmission of ultrathin water sheet samples uniformly heated by a 13.6 nm FEL approaching a highly conducting state at electron temperatures exceeding 20000 K.The experiment probes the trajectory ofwater through the high-energy-density phase space and provides insights into changes in the index of refraction,charge carrier densities,andACelectrical conductivity at optical frequencies.At excitation energy densities exceeding 10MJ/kg,the index of refraction falls to n0.7,and the thermally excited free-carrier density reaches ne531027 m−3,which is over an order of magnitude higher than that of the electron carriers produced by direct photoionization.Significant specular reflection is observed owing to critical electron density shielding of electromagnetic waves.Themeasured optical conductivity reaches 23104 S/m,a value that is one to two orders of magnitude lower than those of simplemetals in a liquid state.At electron temperatures below 15000 K,the experimental results agreewell with the theoretical calculations using density-functional theory/molecular-dynamics simulations.With increasing temperature,the electron density increases and the system approaches a Fermi distribution.In this regime,the conductivities agree better with predictions from the Ziman theory of liquid metals.
文摘A quantum spin liquid (QSL) is an exotic quantum ground state that does not break conventional symmetries and where the spins in the system remain dynamic down to zero temperature. Unlike a trivial paramagnetic state, it features long-range quantum entanglement and supports fractionalized excitations.
基金Project supported by U.S.Department of Energy,Office of Science,Office of Basic Energy Sciences under Contract No.DE-AC02-76SF00515National Science Foundation under Grant No.DMR-1832613.
文摘The hierarchical structure of the composite cathodes brings in significant chemical complexity related to the interfaces,such as cathode electrolyte interphase.These interfaces account for only a small fraction of the volume and mass,they could,however,have profound impacts on the cell-level electrochemistry.As the investigation of these interfaces becomes a crucial topic in the battery research,there is a need to properly study the surface chemistry,particularly to eliminate the biased,incomplete characterization provided by techniques that assume the homogeneous surface chemistry.Herein,we utilize nano-resolution spatially-resolved x-ray spectroscopic tools to probe the heterogeneity of the surface chemistry on LiNi0.8Mn0.1Co0.1O2 layered cathode secondary particles.Informed by the nano-resolution mapping of the Ni valance state,which serves as a measurement of the local surface chemistry,we construct a conceptual model to elucidate the electrochemical consequence of the inhomogeneous local impedance over the particle surface.Going beyond the implication in battery science,our work highlights a balance between the high-resolution probing the local chemistry and the statistical representativeness,which is particularly vital in the study of the highly complex material systems.
基金the financial support by the Natural Science Foundation of China(22172167)the Senior Talent Startup Funds of Jiangsu University(4111310024)。
文摘In this work,a one-pot strategy is presented to directly synthesize amorphous Fe_(x)Ni_(y) hydroxide nanoclusters(denoted as ANC-Fe_(x)Ni_(y),<2 nm)with oxygen vacancies induced by ionic liquids.The ANC-Fe_(x)Ni_(y) catalyst presents abundant catalytic sites and high intrinsic conductivity.As such,the optimized ANC-Fe_(1)Ni_(2) exhibits high activity in oxygen evolution reaction(OER)with a Tafel slope of 39 m V dec^(–1) and an overpotential of 266 m V at 10 m A cm^(-2).Notably,the optimized ANC-Fe_(1)Ni_(2) shows an extraordinarily large mass activity of 3028 Ag_(FeNi)^(–1) at the overpotential of 300 m V,which is~24-fold of commercial RuO_(2) catalyst.The superior activity of these Fe_(x)Ni_(y) hydroxide nanoclusters is ascribed to(i)the amorphous and distorted structure with abundant oxygen vacancies,and(ii)enhanced active site density by downsizing the ANC-FexNiyclusters.This strategy provides a novel route for enhancing OER electrocatalytic performance and highly encouraging for the future application of amorphous metal hydroxides in catalysis.
基金This work was supported by NNSA cooperative Agreement Grant No.DE-NA0002008the DARPA PULSE program(No.12-63-PULSE-FP014)+2 种基金the Air Force Office of Scientific Research(Grant No.FA9550-14-1-0045)This work was performed under the auspices of the U.S.Department of Energy by the Triad National Security,LLC(Contract No.89233218CNA000001)Los Alamos National Laboratory and was supported by the LANL Office of Experimental Sciences programs.Simulations were run on the LANL Institutional Computing Clusters.
文摘An experimental and simulation study of warm dense carbon foams at ambient density(ne∼10^(21) cm^(−3))is presented.This study of isochorically heated foams is motivated by their potential application in carbon-atmosphere white-dwarf envelopes,where there are modeling uncertainties due to the equation of state.The foams are heated on an approximately picosecond time scale with a laser-accelerated proton beam.The cooling and expansion of the heated foams can be modeled with appropriately initialized radiation-hydrodynamics codes;xRAGE code is used in this work.The primary experimental diagnostic is the streaked optical pyrometer,which images a narrow band of radiation from the rear surface of the heated material.Presented are xRAGE modeling results for both solid aluminum targets and carbonized resorcinol-formaldehyde foam targets,showing that the foam appears to cool slowly on the pyrometer because of partial transparency.So that simulations of cooling foam are processed properly,it is necessary to account for finite optical depth in the photosphere calculation,and the methods for performing that calculation are presented in depth.
文摘Who/what inspires you to the field of energy and nanomaterials?My Ph.D advisor Professor Charles Lieber has been a big inspiration to me since my graduate school study.I was later influenced quite a bit by my postdoctoral mentor Professor Paul Alivisatos.By the end of my postdoctoral study in 2005,I was also influenced by Professor Steven Chu,who is a major figure to excite me to go into the energy area.I have many on‐going collaborations with Professor Chu.
基金Project supported by the Department of Energy,Office of Basic Energy Sciences(Grant No.DE-AC02-76SF00515)
文摘Recently, the quasi-two-dimensional electron gas (q2DEG) confined at the interface between LaAlO3 and SrTiO3 has attracted significant attention. In this paper, we briefly review experimental methods that have been used to tune the carrier density and mobility of this q2DEG. These methods can be classified into two categories: growth-related tuning (i.e. substrate, growth temperature, oxygen pressure, post-annealing, LaAlO3 thickness, stoichiometry, and capping layers) and post-growth tuning (i.e. electrostatic field gating, conductive atomic force microscopy and surface adsorbates). Taken together, these methods enable the broad tuning of the electronic properties of this interface.
文摘Owing to their ultra-high accelerating gradients,combined with injection inside micrometer-scale accelerating wakefield buckets,plasma-based accelerators hold great potential to drive a new generation of free-electron lasers(FELs).Indeed,the first demonstration of plasma-driven FEL gain was reported recently,representing a major milestone for the field.Several groups around the world are pursuing these novel light sources,with methodology varying in the use of wakefield driver(laser-driven or beam-driven),plasma structure,phase-space manipulation,beamline design,and undulator technology,among others.This paper presents our best attempt to provide a comprehensive overview of the global community efforts towards plasma-based FEL research and development.
文摘To be useful for most scientific and medical applications,compact particle accelerators will require much higher average current than enabled by current architectures.For this purpose,we propose a photonic crystal architecture for a dielectric laser accelerator,referred to as a multi-input multi-output silicon accelerator(MIMOSA),that enables simultancous acceleration of multiple electron beams,increasing the total electron throughput by at least I order of magnitude.To achieve this,we show that the photonic crystal must support a mode at the I point in reciprocal space,with a normalized frequency equal to the normalized speed of the phase-matched electron.We show that the figure of merit of the MIMOSA can be inferred from the eigenmodes of the corresponding infinitely periodic structure,which provides a powerful approach to design such devices.Additionally,we extend the MIMOSA architecture to electron deflectors and other clectron manipulation functionalities.These additional functionalities,combined with the increased electron throughput of these devices,permit all-optical on-chip manipulation of electron beams in a fully integrated architecture compatible with current fabrication technologies,which opens the way to unconventional electron beam shaping,imaging,and radiationg encration.