Atomic spin gyroscopes are promising candidates for next-generation inertial navigation due to extremely high theoretical precision,relatively small size among atomic gyroscopes,and promising potential for miniaturiza...Atomic spin gyroscopes are promising candidates for next-generation inertial navigation due to extremely high theoretical precision,relatively small size among atomic gyroscopes,and promising potential for miniaturization.In particular,the spin-exchange relaxation-free(SERF)atomic gyroscope relies on optical pumping to polarize atoms,enabling rotation sensing through the Faraday optical rotation angle(FORA).However,fluctuations in atomic density introduce systematic errors in FORA measurements,limiting long-term stability.We present a data-driven decoupling method that isolates atomic density fluctuations from the FORA signal by modeling spatially resolved light absorption in the vapor cell.The model accounts for the spatial distribution of spin polarization in the pump-light interaction volume,density-dependent relaxation rates,wall-induced relaxation,and polarization diffusion,and is implemented within a finite-element framework.Compared to the conventional Lambert-Beer law,which assumes one-dimensional homogeneity,our approach captures the full threedimensional density and polarization distribution,significantly improving the accuracy of light absorption modeling.The resulting absorption-density maps are used to train a feedforward neural network,yielding a high-precision estimator for atomic density fluctuations.This estimator enables the construction of a decoupling equation that separates the density contribution from the FORA signal.Experimental validation shows that this method improves the bias instability atσ(100 s)of the gyroscope was improved by 73.1%compared to traditional platinum-resistance-based stabilization.The proposed framework is general and can be extended to other optical pumping-based sensors,such as optically pumped magnetometers.展开更多
In this article,we introduce a new theoretical approach to improve the accuracy of twodimensional(2D)atomic localization within a tripod-type,four-level atomic system by analyzing its transmission spectrum.In this met...In this article,we introduce a new theoretical approach to improve the accuracy of twodimensional(2D)atomic localization within a tripod-type,four-level atomic system by analyzing its transmission spectrum.In this method,the atom interacts with two orthogonal standing-wave fields and a weak probe field.By examining how the weak probe field passes through the system,we can determine the atom position.Our analysis reveals the presence of both double and sharply defined single localized peaks in the transmission spectrum,which correspond to specific positions of the atom.Importantly,we achieve ultra-high-resolution atomic localization with accuracy confined to a region smaller thanλ/32×λ/32.This level of precision is a significant improvement compared to earlier methods,which had lower localization accuracy.The increased precision is due to the complex interaction between the atom and the carefully controlled standing-wave and probe fields,which allows for precise control over the atom's position.The implications of this work are significant,especially for applications like nano-lithography,where precise atomic placement is essential,and for laser cooling technologies,where better atomic localization could lead to more effective cooling processes and improved manipulation of atomic states.展开更多
We propose a novel cooling protocol within a triple-Laguerre-Gaussian cavity optomechanical system,which is designed to suppress the thermal vibrations of a rotating mirror to reach its quantum ground state.The system...We propose a novel cooling protocol within a triple-Laguerre-Gaussian cavity optomechanical system,which is designed to suppress the thermal vibrations of a rotating mirror to reach its quantum ground state.The system incorporates two auxiliary cavities and an atomic ensemble coupled to a Laguerre-Gaussian rotational cavity.By carefully selecting system parameters,the cooling process of the rotating mirror is significantly enhanced,while the heating process is effectively suppressed,enabling efficient ground-state cooling even in the unresolved sideband regime.Compared to previous works,our scheme reduces the stringent restrictions on auxiliary systems,making it more experimentally feasible under broader parameter conditions.These findings provide a robust approach for achieving ground-state cooling in mechanical resonators.展开更多
Rydberg-atom-based superheterodyne receivers integrate self-calibration,high sensitivity,a wide operational frequency range,and phase/frequency resolved detection capabilities,demonstrating broad application prospects...Rydberg-atom-based superheterodyne receivers integrate self-calibration,high sensitivity,a wide operational frequency range,and phase/frequency resolved detection capabilities,demonstrating broad application prospects as nextgeneration microwave receivers.Linear gain and linear dynamic range(LDR)are critical metrics for assessing receiver sensitivity and demodulation fidelity,respectively.We numerically solve the four-level master equation and then employ particle swarm optimization(PSO)algorithm to co-optimize linear gain and LDR in atomic superheterodyne receivers based on balanced homodyne detection.Further,we systematically account for dominant dephasing mechanisms in the simulation,encompassing spontaneous decay,transit dephasing,collision dephasing,laser linewidth dephasing,and Doppler averaging.Homodyne readout utilizes both the real and imaginary parts of polarizability for sensing.In the case of the photon shot noise limit,its signal-to-noise ratio(SNR)expression resembles that of direct optical-intensity readout.However,the inherent coherent subtraction operation in homodyne detection significantly suppresses common-mode noise,while appropriately increasing the reference beam power enhances the gain in practical experiments.Indeed,this co-optimization problem,characterized by a high-dimensional variable space,two objectives,and non-convexity,is well-suited for solution by PSO.In addition,probe and coupling detuning contribute equivalently to polarizability and compensate for each other owing to Doppler averaging,thereby reducing the optimization variable space by one.By adopting a product form of linear gain and LDR as the fitness function,the PSO achieves rapid convergence.Here,the effectiveness of the PSO results is verified via the total harmonic distortion(THD).The relative error-based LDR calculation method we proposed efficiently measures receiver response linearity with consuming fewer computational resources.This research is expected to offer valuable insights into enhancing the performance of Rydberg-atom-based superheterodyne receivers.展开更多
Inorganic perovskites,a class of materials with the general formula ABX3,exhibit a wide range of electronic,dielectric,and structural properties,making them pivotal in energy,electronics,and catalysis applications.Acc...Inorganic perovskites,a class of materials with the general formula ABX3,exhibit a wide range of electronic,dielectric,and structural properties,making them pivotal in energy,electronics,and catalysis applications.Accurate atomistic simulations of these materials require accurate interatomic potentials that capture both short-range and long-range interactions.While first-principles methods are of high accuracy,empirical and machine learning potentials remain essential for large-scale simulations.This survey categorizes and reviews the atomic potentials used in inorganic perovskite modeling based on how they treat electrostatic interactions:potentials without charges,potentials with constant charges,and potentials with variable charges.Given the ionic nature of perovskites,we emphasize the importance of charge treatment,and each class of potentials is discussed in detail with representative examples,functional forms,and application scenarios.For comparison,we perform molecular dynamics simulations to calculate the critical temperature for the phase transition of the perovskite CsPbI_(3) with available empirical potentials,highlighting their strengths and limitations in capturing structural evolution.Finally,we outline future directions for developing more accurate and transferable atomic potentials for inorganic perovskites.We hope that this review can serve as a guiding resource for researchers who are starting to perform simulations for inorganic perovskites.展开更多
Chlorinated antibiotics pose great challenges in efficient removal,while for the first time,this work greatly enhanced their electrocatalytic dechlorination performance by construction of non-noble metal Co_(3)O_(4)/g...Chlorinated antibiotics pose great challenges in efficient removal,while for the first time,this work greatly enhanced their electrocatalytic dechlorination performance by construction of non-noble metal Co_(3)O_(4)/g-C_(3)N_(4) heterojunctions to improve process cost-effectiveness.The Co_(3)O_(4)/g-C_(3)N_(4) heterojunction demonstrated an effective removal of 93.6%thiamphenicol(TAP)within 45 min,with the rate constant(0.0584 min^(-1))that was 2.4 and 2.8 times that of Co_(3)O_(4) and g-C_(3)N_(4) alone,respectively.The formation of heterojunctions facilitated electron transfer,enriched the electron density on Co_(3)O_(4),and enhanced the adsorption of pollutants as well as the desorption of degradation intermediates.The enhanced production of atomic hydrogen(H*)of Co_(3)O_(4)/g-C_(3)N_(4),which increased by 13.6-28.2 times,contributed more to pollutant removal(64.0%),much higher than that of Co_(3)O_(4)(37.3%)and g-C_(3)N_(4)(6.1%).The energy barrier for H_(2) formation on Co_(3)O_(4)/g-C_(3)N_(4)(0.75 eV)was higher than that on Co_(3)O_(4)(-1.84 eV),supporting that it could stabilize H*and inhibit the formation of H_(2).The Co_(3)O_(4)/g-C_(3)N_(4) heterojunction exhibited stable performance with less impact by pH and co-existing ions,and posed effectiveness for the dechlorination of typical chlorinated antibiotics.This study offers an efficient and sustainable strategy for constructing heterojunctions to enhance the performance of non-noble metal catalysts in electrocatalytic dechlorination.展开更多
Atomic layer deposition(ALD)is extensively used to fabricate doped dielectrics due to its ability to deposit conformal films with atomic-scale thickness control.Al-doped TiO_(2)(ATO)is a promising high-k dielectric fo...Atomic layer deposition(ALD)is extensively used to fabricate doped dielectrics due to its ability to deposit conformal films with atomic-scale thickness control.Al-doped TiO_(2)(ATO)is a promising high-k dielectric for dynamic random access memory(DRAM)applications,offering a high dielectric constant with a remarkable leakage-lowering effect by Al acceptor doping.However,ATO fabrication via conventional supercycle-based ALD suffers from severe crystallinity loss during the growth of TiO_(2) upon Al doping owing to the dopant-induced lattice disorder.In addition,Al doping cannot reduce any inherent O vacancies(V_(O))of TiO_(2),although the original purpose of doping was to address the n-type nature caused by V_(O).To resolve these limitations,we propose a single-step,in-situ Ar/O_(2) post-doping plasma(PDP)process immediately after the Al dopant incorporation.Using the PDP process,simultaneous atomic-scale dopant migration-mediated crystallization and V_(O) annihilation were successfully initiated.Thus,the surface concentration of the dopant decreased,reducing the dopant-induced lattice distortion,while promoting the highly crystallized seed layer-like surface.Consequently,strong rutile-phase recovery was accompanied by enhanced lattice-matched growth.In addition,the PDP process significantly lowers the V_(O)-to-lattice oxygen ratio by facilitating the recombination between reactive O species and V_(O),increasing the corresponding 0.4 e V of conduction band offset(CBO).Despite the common trade-off between the dielectric constant and leakage,the Pt/PDP-ATO/Ru capacitor exhibited a simultaneous 30%increase in dielectric constant and up to a 1.6-order reduction in leakage current density.展开更多
Single-atom catalysts(SACs)have demonstrated excellent performance in heterogeneous catalytic reactions owing to their maximized atomic efficiency,distinctive geometric,and electronic configurations.However,the effica...Single-atom catalysts(SACs)have demonstrated excellent performance in heterogeneous catalytic reactions owing to their maximized atomic efficiency,distinctive geometric,and electronic configurations.However,the efficacy of SACs remains limited for certain reactions requiring simultaneous activation of multiple reactants over metallic active sites.Herein,we report an atomically dispersed Pt1Ru1 dual-atom pair site anchored on nanodiamond@graphene(ND@G)for CO oxidation.The Pt1Ru1 dual-atom catalyst shows an exceptional turnover frequency(TOF)of 17.6.10^(-2)s^(-1)at significantly lower temperature(30℃),achieving a tenfold increase in TOF compared to singleatom Pt1/ND@G catalyst(1.5.10^(-2)s^(-1))and surpassing to previously reported Pt-based catalysts under similar conditions.Moreover,the catalyst demonstrates excellent stability,maintaining its activity for 40 h at 80℃without significant deactivation.The superior catalytic performance of Pt-Ru dual-atom catalysts is attributed to the synergistic effect between Pt and Ru atoms with enhanced metallicity for improving simultaneous adsorption and activation of CO and O_(2),and the tuning of conventional competitive reactant adsorption into a non-competitive pathway over dual-atom pair sites.The present work manifests the advantages of dual-atom pair sites in heterogeneous catalysis and paves the way for precise design of catalysts at the atomic scale.展开更多
Oxide semiconductors(OSs),introduced by the Hosono group in the early 2000s,have evolved from display backplane materials to promising candidates for advanced memory and logic devices.The exceptionally low leakage cur...Oxide semiconductors(OSs),introduced by the Hosono group in the early 2000s,have evolved from display backplane materials to promising candidates for advanced memory and logic devices.The exceptionally low leakage current of OSs and compatibility with three-dimensional(3D)architectures have recently sparked renewed interest in their use in semiconductor applications.This review begins by exploring the unique material properties of OSs,which fundamentally originate from their distinct electronic band structure.Subsequently,we focus on atomic layer deposition(ALD),a core technique for growing excellent OS films,covering both basic and advanced processes compatible with 3D scaling.The basic surface reaction mechanisms—adsorption and reaction—and their roles in film growth are introduced.Furthermore,material design strategies,such as cation selection,crystallinity control,anion doping,and heterostructure engineering,are discussed.We also highlight challenges in memory applications,including contact resistance,hydrogen instability,and lack of p-type materials,and discuss the feasibility of ALD-grown OSs as potential solutions.Lastly,we provide an outlook on the role of ALD-grown OSs in memory technologies.This review bridges material fundamentals and device-level requirements,offering a comprehensive perspective on the potential of ALD-driven OSs for next-generation semiconductor memory devices.展开更多
The development of atomically dispersed multi-metallic catalysts is imperative for tailoring catalytic performance and elucidating structure-activity relationships.However,synthesizing such precisely engineered archit...The development of atomically dispersed multi-metallic catalysts is imperative for tailoring catalytic performance and elucidating structure-activity relationships.However,synthesizing such precisely engineered architectures while maintaining atomic dispersion of distinct metal centers remains a formidable challenge due to thermodynamic instability and synthetic complexity.We herein propose a topological confinement pre-anchoring strategy via pre-anchoring spatially resolved Zn/Fe dual-metal sources in a structurally engineered metal-organic framework precursor to synthesize atomically dispersed ZnFe bimetallic single-atom catalysts.Extended X-ray absorption fine structure measurements and X-ray absorption near-edge structure reveal that the atomically dispersed Zn/Fe metal sites and electronic redistribution in ZnFe bimetallic single-atom catalysts.The ultrahigh surface area,hierarchical pore,and synergistic effect between Zn/Fe can greatly favor the exposure of the active site,mass transport,and improvement of intrinsic activity.Consequently,the ZnFe bimetallic single-atom catalyst demonstrates superior oxygen reduction reaction performance,achieving a half-wave potential of 0.86 V and delivering a kinetic current density of 10.1 mA cm^(-2)at 0.85 V versus RHE in 0.1 m KOH electrolyte.These metrics not only surpass those of commercial Pt/C,but also rival the highest-performing catalysts reported to date.The Zn-air battery built with ZnFe bimetallic single-atom catalyst exhibits high power density(278.5 mW cm^(-2))and specific discharging capacities(657 mAh g^(-1)).This work provides a new design pathway for constructing atomically dispersed multi-metal electrocatalysts for high-performance energy-related applications.展开更多
Heat dissipation highly relies on the thermal conductivity(κ)of materials.Materials with large bandgaps and signifcant atomic mass ratios,such as BAs,SiC,andθ-TaN,have attracted considerable attention due to their p...Heat dissipation highly relies on the thermal conductivity(κ)of materials.Materials with large bandgaps and signifcant atomic mass ratios,such as BAs,SiC,andθ-TaN,have attracted considerable attention due to their potential for achieving ultra-highκ,with BAs serving as a particularly representative example due to its unique combination of large bandgap and high thermal conductivity.In this paper,the efects of atomic mass modifcation on phonon bandgap andκare systematically investigated using a BAs model,accounting for both three-and four-phonon scattering processes.A 20%increase inκcan be obtained by substituting B,achieved through widening the phonon bandgap,which suppresses phonon scattering.Notably,the AAOO four-phonon scattering channel is more suppressed than the AAO three-phonon channel,leading to an increased phonon lifetime(τ).For As,κcan also be enhanced by 5%when replaced by lighter atoms,such as^(69)As,primarily due to the increased phonon group velocity(υ).We systematically clarify how atomic-mass-induced bandgap variations afectτ,υ,and thereforeκin wide-bandgap systems.Our work provides a specifc scheme for further improving the ultra-highκof materials with large bandgaps,which possesses great guiding signifcance.展开更多
The powerful light field manipulation capability of metasurfaces offers a novel development perspective for the quantum precision measurement.By applying the phasegradient metasurface(PGM)to atomic magnetometers(AMs),...The powerful light field manipulation capability of metasurfaces offers a novel development perspective for the quantum precision measurement.By applying the phasegradient metasurface(PGM)to atomic magnetometers(AMs),we have proposed and experimentally demonstrated a new type of compact single-beam elliptically polarized atomic magnetometers(EPAMs).Employing the fabricated chiral beam splitter PGM with high cross-polarization transmittance,a new atomic spin chirality detection method was devised,enabling the ultra-high sensitivity for extremely weak magnetic field measurement and achieving a high sensitivity of 2.67 pT/Hz^(1/2)under an external magnetic field of approximately 10,000 nT.The new AMs combine the pumping and probing polarized light,achieving a compact design.The fabricated PGM has a size of only 3 mm×3 mm×0.7 mm,which is beneficial for the miniaturization and integration of AMs.This work effectively expands the application of metasurfaces in the field of quantum precision measurement,and also provides a new viewpoint for the design and development of high-sensitivity and miniaturized AMs.展开更多
A research team led by Prof.YANG Kai at the Institute of Physics(IOP),Chinese Academy of Sciences,in collaboration with Prof.FERNÁNDEZ-ROSSIER Joaquín from International Iberian Nanotechnology Laboratory,has...A research team led by Prof.YANG Kai at the Institute of Physics(IOP),Chinese Academy of Sciences,in collaboration with Prof.FERNÁNDEZ-ROSSIER Joaquín from International Iberian Nanotechnology Laboratory,has demonstrated all-electrical control of quantum interference in individual atomic spins on a surface,opening new possibilities for fast and robust quantum-state manipulation at the atomic scale.展开更多
Single-atom catalysts (SACs) have emerged as a transformative class of materials in heterogeneous catalysis owing to their atomically dispersed metal centers, maximal atom utilization, and well-defined coordination en...Single-atom catalysts (SACs) have emerged as a transformative class of materials in heterogeneous catalysis owing to their atomically dispersed metal centers, maximal atom utilization, and well-defined coordination environments. In the energy sector, SACs have shown exceptional performance in electrocatalytic reactions such as the oxygen reduction reaction (ORR), hydrogen evolution reaction (HER), and carbon dioxide reduction (CO_(2)RR), where their tunable local electronic structures facilitate high activity and selectivity under mild conditions. Meanwhile, in the environmental domain, SACs are increasingly explored for advanced oxidation processes (AOPs), particularly in water purification applications, due to their ability to generate reactive species from green oxidants like hydrogen peroxide or peroxymonosulfate (PMS). Among various AOP strategies, PMS-based Fenton-like reactions have gained attention due to the high oxidation potential and stability of PMS in a wide pH range.展开更多
Aberration-corrected annular dark-field scanning transmission electron microscopy(ADF-STEM)is a powerful tool for structural and chemical analysis of materials.Conventional analyses of ADF-STEM images rely on human la...Aberration-corrected annular dark-field scanning transmission electron microscopy(ADF-STEM)is a powerful tool for structural and chemical analysis of materials.Conventional analyses of ADF-STEM images rely on human labeling,making them labor-intensive and prone to subjective error.Here,we introduce a deep-learning-based workflow combining a pix2pix network for image denoising and either a mathematical algorithm local intensity threshold segmentation(LITS)or another deep learning network UNet for chemical identification.After denoising,the processed images exhibit a five-fold improvement in signal-to-noise ratio and a 20%increase in accuracy of atomic localization.Then,we take atomic-resolution images of Y–Ce dual-atom catalysts(DACs)and Fe-doped ReSe_(2) nanosheets as examples to validate the performance.Pix2pix is applied to identify atomic sites in Y–Ce DACs with a location recall of 0.88 and a location precision of 0.99.LITS is used to further differentiate Y and Ce sites by the intensity of atomic sites.Furthermore,pix2pix and UNet workflow with better automaticity is applied to identification of Fe-doped ReSe_(2) nanosheets.Three types of atomic sites(Re,the substitution of Fe for Re,and the adatom of Fe on Re)are distinguished with the identification recall of more than 0.90 and the precision of higher than 0.93.These results suggest that this strategy facilitates high-quality and automated chemical identification of atomic-resolution images.展开更多
Single-atom Fe catalysts show significant promise in the electrocatalytic reduction of CO_(2)(CO_(2)RR),while their performance remains inferior to that of precious metal catalysts due to the overly strong binding of^...Single-atom Fe catalysts show significant promise in the electrocatalytic reduction of CO_(2)(CO_(2)RR),while their performance remains inferior to that of precious metal catalysts due to the overly strong binding of^(*)CO intermediates.Although the introduction of heteroatoms or transition metal sites can modulate the binding strength of^(*)CO on Fe sites,these regulators often induce competitive hydrogen evolution reaction(HER)with reduced Faraday efficiency(FE).In this work,we employ HER-inert Sn as a regulator to tune the electronic structure of Fe,weakening^(*)CO adsorption and enhancing CO_(2)RR performance.Diatomic Fe-Sn pairs supported on N-doped carbon(Fe-Sn/NC)were synthesized,achieving FE for CO exceeding 90%over a broad potential range from−0.4 to−0.9 V versus the reversible hydrogen electrode.Fe-Sn/NC shows a high turnover frequency of 1.5×10^(4)h^(-1),much higher than that of Fe/NC.Characterization results and theoretical calculations demonstrate that bonding Sn site to Fe generates electron-rich Fe centers,effectively reducing the adsorption strength of^(*)CO without triggering HER.Additionally,Fe-Sn/NC exhibits exceptional activity in hydrazine oxidation performance(HzOR).The HzOR-assisted CO_(2)RR system using Fe-Sn/NC as electrodes reduces energy consumption by 38%compared with the conventional CO_(2)RR coupled oxygen evolution reaction system.展开更多
The T_(1)(Al_(2) CuLi)phase is one of the most effective strengthening nanoscale-precipitate in Al-Cu alloys with Li.However,its formation and evolution still need to be further clarified during aging due to the compl...The T_(1)(Al_(2) CuLi)phase is one of the most effective strengthening nanoscale-precipitate in Al-Cu alloys with Li.However,its formation and evolution still need to be further clarified during aging due to the complex precipitation sequences.Here,a detailed investigation has been carried out on the atomic struc-tural evolution of T_(1) precipitate in an aged Al-Cu-Li-Mg-Ag alloy using state-of-the-art Cs-corrected high-angle annular dark field(HAADF)-coupled with integrated differential phase contrast(iDPC)-scanning transmission electron microscopy(STEM)and energy-dispersive X-ray spectroscopy(EDXS)techniques.An intermediate T_(1)’phase between T_(1p) and T_(1) phase,with a crystal structure and orientation rela-tionship consistent with T_(1),but exhibiting different atomic occupancy and chemical composition was found.We observed the atomic structural transformation from T_(1p) to T_(1)’phase(fcc→hcp),involving only 1/12<112>Al shear component.DFT calculation results validated our proposed structural models and the precipitation sequence.Besides,the distributions of minor solute elements(Ag,Mg,and Zn)in the pre-cipitates exhibited significant differences.These findings may contribute to a further understanding of the nucleation mechanism of T_(1) precipitate.展开更多
Metal-based catalysts are prevalent in the CO_(2) hydrogenation to methanol owing to their remarkable catalytic activity.Herein,Ru/In_(2)O_(3) catalysts with different morphologies obtained by doping Ru into In_(2)O_(...Metal-based catalysts are prevalent in the CO_(2) hydrogenation to methanol owing to their remarkable catalytic activity.Herein,Ru/In_(2)O_(3) catalysts with different morphologies obtained by doping Ru into In_(2)O_(3) with irregular,rod-like,and flower-like morphologies are used for catalytic CO_(2) hydrogenation to methanol.Results indicate that the flower-like Ru/In_(2)O_(3)(Ru/In_(2)O_(3)-F)exhibits higher catalytic performance than Ru/In_(2)O_(3) with other morphologies,achieving a 12.9%CO_(2) conversion,74.02%methanol selectivity,and 671.36 mg_(MeOH) h^(−1) g_(cat)^(−1) methanol spatiotemporal yield.Furthermore,Ru/In_(2)O_(3)-F maintains its catalytic stability over 200 h at 5 MPa and 290℃.The promotional effect mainly stems from the fact that electronic structure of Ru can be effectively adjusted by modulating the morphology of In_(2)O_(3).The strong interaction between atomically dispersed Ru and In_(2)O_(3)-F enhances the structural stability of Ru,inhibiting the agglomeration of the catalyst during the reaction process.Furthermore,density-functional theory calculations reveal that highly dispersed Ru atoms not only perform efficient and rapid electronic gain and loss processes,facilitating the catalytic activation of H_(2) into H intermediates.It also enables the generated reactive H to rapidly overflow to the surrounding In sites to participate in CO_(2) reduction.These findings provide a theoretical basis for the development of high-performance catalysts for CO_(2) hydrogenation.展开更多
Atomic surfaces are strictly required by high-performance devices of diamond.Nevertheless,diamond is the hardest material in nature,leading to the low material removal rate(MRR)and high surface roughness during machin...Atomic surfaces are strictly required by high-performance devices of diamond.Nevertheless,diamond is the hardest material in nature,leading to the low material removal rate(MRR)and high surface roughness during machining.Noxious slurries are widely used in conventional chemical mechanical polishing(CMP),resulting in the possible pollution to the environment.Moreover,the traditional slurries normally contain more than four ingredients,causing difficulties to control the process and quality of CMP.To solve these challenges,a novel green CMP for single crystal diamond was developed,consisting of only hydrogen peroxide,diamond abrasive and Prussian blue(PB)/titania catalyst.After CMP,atomic surface is achieved with surface roughness Sa of 0.079 nm,and the MRR is 1168 nm·h^(-1).Thickness of damaged layer is merely 0.66 nm confirmed by transmission electron microscopy(TEM).X-ray photoelectron spectroscopy,electron paramagnetic resonance and TEM reveal that·OH radicals form under ultraviolet irradiation on PB/titania catalyst.The·OH radicals oxidize diamond,transforming it from monocrystalline to amorphous atomic structure,generating a soft amorphous layer.This contributes the high MRR and formation of atomic surface on diamond.The developed novel green CMP offers new insights to achieve atomic surface of diamond for potential use in their high-performance devices.展开更多
Broadband transparent films play a pivotal role in various applications such as lenses and solar cells,particularly porous structured transparent films exhibit significant potential.This study investigates a porous Si...Broadband transparent films play a pivotal role in various applications such as lenses and solar cells,particularly porous structured transparent films exhibit significant potential.This study investigates a porous SiO_(2) refractive index gradient anti-reflective film prepared by atomic layer deposition(ALD).A porous SiO_(2) film with gradual porosity was obtained by phosphoric acid etching of Al_(2)O_(3)/SiO_(2) multilayers with gradient Al2O3 ratios,achieving a gradual decrease in refractive index from the substrate to the surface.The film exhibited an average transmittance as high as 97.8%within the wavelength range from 320 nm to 1200 nm.The environmental adaptability was further enhanced by surface modification using rare earth oxide(REO)La_(2)O_(3),resulting in formation of a lotus leaf-like structure and achieving a water contact angle of 100.0°.These data proved that the modification significantly improved hydrophobic self-cleaning capability while maintaining exceptional transparency of the film.The surface structure of the modified film remained undamaged even after undergoing wipe testing,demonstrating its excellent surface durability.展开更多
基金supported by the Beijing Natural Science Foundation(Grant No.3252013)the Innovation Program for Quantum Science and Technology(Grant No.2021ZD0300402)+1 种基金the National Natural Science Foundation of China(Grant No.61673041)Key Area Research and Development Program of Guangdong Province(Grant No.2021B0101410005)。
文摘Atomic spin gyroscopes are promising candidates for next-generation inertial navigation due to extremely high theoretical precision,relatively small size among atomic gyroscopes,and promising potential for miniaturization.In particular,the spin-exchange relaxation-free(SERF)atomic gyroscope relies on optical pumping to polarize atoms,enabling rotation sensing through the Faraday optical rotation angle(FORA).However,fluctuations in atomic density introduce systematic errors in FORA measurements,limiting long-term stability.We present a data-driven decoupling method that isolates atomic density fluctuations from the FORA signal by modeling spatially resolved light absorption in the vapor cell.The model accounts for the spatial distribution of spin polarization in the pump-light interaction volume,density-dependent relaxation rates,wall-induced relaxation,and polarization diffusion,and is implemented within a finite-element framework.Compared to the conventional Lambert-Beer law,which assumes one-dimensional homogeneity,our approach captures the full threedimensional density and polarization distribution,significantly improving the accuracy of light absorption modeling.The resulting absorption-density maps are used to train a feedforward neural network,yielding a high-precision estimator for atomic density fluctuations.This estimator enables the construction of a decoupling equation that separates the density contribution from the FORA signal.Experimental validation shows that this method improves the bias instability atσ(100 s)of the gyroscope was improved by 73.1%compared to traditional platinum-resistance-based stabilization.The proposed framework is general and can be extended to other optical pumping-based sensors,such as optically pumped magnetometers.
基金Princess Nourah bint Abdulrahman University Researchers Supporting Project number(PNURSP2025R8)。
文摘In this article,we introduce a new theoretical approach to improve the accuracy of twodimensional(2D)atomic localization within a tripod-type,four-level atomic system by analyzing its transmission spectrum.In this method,the atom interacts with two orthogonal standing-wave fields and a weak probe field.By examining how the weak probe field passes through the system,we can determine the atom position.Our analysis reveals the presence of both double and sharply defined single localized peaks in the transmission spectrum,which correspond to specific positions of the atom.Importantly,we achieve ultra-high-resolution atomic localization with accuracy confined to a region smaller thanλ/32×λ/32.This level of precision is a significant improvement compared to earlier methods,which had lower localization accuracy.The increased precision is due to the complex interaction between the atom and the carefully controlled standing-wave and probe fields,which allows for precise control over the atom's position.The implications of this work are significant,especially for applications like nano-lithography,where precise atomic placement is essential,and for laser cooling technologies,where better atomic localization could lead to more effective cooling processes and improved manipulation of atomic states.
基金Project supported by the National Natural Science Foundation of China(Grant No.62471180)。
文摘We propose a novel cooling protocol within a triple-Laguerre-Gaussian cavity optomechanical system,which is designed to suppress the thermal vibrations of a rotating mirror to reach its quantum ground state.The system incorporates two auxiliary cavities and an atomic ensemble coupled to a Laguerre-Gaussian rotational cavity.By carefully selecting system parameters,the cooling process of the rotating mirror is significantly enhanced,while the heating process is effectively suppressed,enabling efficient ground-state cooling even in the unresolved sideband regime.Compared to previous works,our scheme reduces the stringent restrictions on auxiliary systems,making it more experimentally feasible under broader parameter conditions.These findings provide a robust approach for achieving ground-state cooling in mechanical resonators.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.62331024 and 62571549)the National Key Research and Development Program of China(Grant No.2022YFB2802804)。
文摘Rydberg-atom-based superheterodyne receivers integrate self-calibration,high sensitivity,a wide operational frequency range,and phase/frequency resolved detection capabilities,demonstrating broad application prospects as nextgeneration microwave receivers.Linear gain and linear dynamic range(LDR)are critical metrics for assessing receiver sensitivity and demodulation fidelity,respectively.We numerically solve the four-level master equation and then employ particle swarm optimization(PSO)algorithm to co-optimize linear gain and LDR in atomic superheterodyne receivers based on balanced homodyne detection.Further,we systematically account for dominant dephasing mechanisms in the simulation,encompassing spontaneous decay,transit dephasing,collision dephasing,laser linewidth dephasing,and Doppler averaging.Homodyne readout utilizes both the real and imaginary parts of polarizability for sensing.In the case of the photon shot noise limit,its signal-to-noise ratio(SNR)expression resembles that of direct optical-intensity readout.However,the inherent coherent subtraction operation in homodyne detection significantly suppresses common-mode noise,while appropriately increasing the reference beam power enhances the gain in practical experiments.Indeed,this co-optimization problem,characterized by a high-dimensional variable space,two objectives,and non-convexity,is well-suited for solution by PSO.In addition,probe and coupling detuning contribute equivalently to polarizability and compensate for each other owing to Doppler averaging,thereby reducing the optimization variable space by one.By adopting a product form of linear gain and LDR as the fitness function,the PSO achieves rapid convergence.Here,the effectiveness of the PSO results is verified via the total harmonic distortion(THD).The relative error-based LDR calculation method we proposed efficiently measures receiver response linearity with consuming fewer computational resources.This research is expected to offer valuable insights into enhancing the performance of Rydberg-atom-based superheterodyne receivers.
基金supported by the National Natural Science Foundation of China(Grant Nos.12072182 and 12421002).
文摘Inorganic perovskites,a class of materials with the general formula ABX3,exhibit a wide range of electronic,dielectric,and structural properties,making them pivotal in energy,electronics,and catalysis applications.Accurate atomistic simulations of these materials require accurate interatomic potentials that capture both short-range and long-range interactions.While first-principles methods are of high accuracy,empirical and machine learning potentials remain essential for large-scale simulations.This survey categorizes and reviews the atomic potentials used in inorganic perovskite modeling based on how they treat electrostatic interactions:potentials without charges,potentials with constant charges,and potentials with variable charges.Given the ionic nature of perovskites,we emphasize the importance of charge treatment,and each class of potentials is discussed in detail with representative examples,functional forms,and application scenarios.For comparison,we perform molecular dynamics simulations to calculate the critical temperature for the phase transition of the perovskite CsPbI_(3) with available empirical potentials,highlighting their strengths and limitations in capturing structural evolution.Finally,we outline future directions for developing more accurate and transferable atomic potentials for inorganic perovskites.We hope that this review can serve as a guiding resource for researchers who are starting to perform simulations for inorganic perovskites.
基金supported by Natural Science Foundation of China(Nos.U23B20165 and 52170085)National Key R&D Program International Cooperation Project(No.2023YFE0108100)+1 种基金Key Project of Natural Science Foundation of Tianjin(No.21JCZDJC00320)Fundamental Research Funds for the Central Universities,Nankai University.
文摘Chlorinated antibiotics pose great challenges in efficient removal,while for the first time,this work greatly enhanced their electrocatalytic dechlorination performance by construction of non-noble metal Co_(3)O_(4)/g-C_(3)N_(4) heterojunctions to improve process cost-effectiveness.The Co_(3)O_(4)/g-C_(3)N_(4) heterojunction demonstrated an effective removal of 93.6%thiamphenicol(TAP)within 45 min,with the rate constant(0.0584 min^(-1))that was 2.4 and 2.8 times that of Co_(3)O_(4) and g-C_(3)N_(4) alone,respectively.The formation of heterojunctions facilitated electron transfer,enriched the electron density on Co_(3)O_(4),and enhanced the adsorption of pollutants as well as the desorption of degradation intermediates.The enhanced production of atomic hydrogen(H*)of Co_(3)O_(4)/g-C_(3)N_(4),which increased by 13.6-28.2 times,contributed more to pollutant removal(64.0%),much higher than that of Co_(3)O_(4)(37.3%)and g-C_(3)N_(4)(6.1%).The energy barrier for H_(2) formation on Co_(3)O_(4)/g-C_(3)N_(4)(0.75 eV)was higher than that on Co_(3)O_(4)(-1.84 eV),supporting that it could stabilize H*and inhibit the formation of H_(2).The Co_(3)O_(4)/g-C_(3)N_(4) heterojunction exhibited stable performance with less impact by pH and co-existing ions,and posed effectiveness for the dechlorination of typical chlorinated antibiotics.This study offers an efficient and sustainable strategy for constructing heterojunctions to enhance the performance of non-noble metal catalysts in electrocatalytic dechlorination.
基金supported by the Samsung Electronics Co.,Ltd.(ISO230414-05954-01)Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(NRF2021R1A6A1A03039981)+2 种基金the Korea Institute for Advancement of Technology(KIAT)Grant,funded by the Korea Government(MOTIE)(P0023703,HRD Program for Industrial Innovation)The computations were performed at the Korea Institute of Science and Technology Information(KISTI)National Supercomputing Center(KSC-2024-CRE-0316)the UNIST Supercomputing Center。
文摘Atomic layer deposition(ALD)is extensively used to fabricate doped dielectrics due to its ability to deposit conformal films with atomic-scale thickness control.Al-doped TiO_(2)(ATO)is a promising high-k dielectric for dynamic random access memory(DRAM)applications,offering a high dielectric constant with a remarkable leakage-lowering effect by Al acceptor doping.However,ATO fabrication via conventional supercycle-based ALD suffers from severe crystallinity loss during the growth of TiO_(2) upon Al doping owing to the dopant-induced lattice disorder.In addition,Al doping cannot reduce any inherent O vacancies(V_(O))of TiO_(2),although the original purpose of doping was to address the n-type nature caused by V_(O).To resolve these limitations,we propose a single-step,in-situ Ar/O_(2) post-doping plasma(PDP)process immediately after the Al dopant incorporation.Using the PDP process,simultaneous atomic-scale dopant migration-mediated crystallization and V_(O) annihilation were successfully initiated.Thus,the surface concentration of the dopant decreased,reducing the dopant-induced lattice distortion,while promoting the highly crystallized seed layer-like surface.Consequently,strong rutile-phase recovery was accompanied by enhanced lattice-matched growth.In addition,the PDP process significantly lowers the V_(O)-to-lattice oxygen ratio by facilitating the recombination between reactive O species and V_(O),increasing the corresponding 0.4 e V of conduction band offset(CBO).Despite the common trade-off between the dielectric constant and leakage,the Pt/PDP-ATO/Ru capacitor exhibited a simultaneous 30%increase in dielectric constant and up to a 1.6-order reduction in leakage current density.
基金supported by the National Key R&D Program of China (2021YFA1502802)the National Natural Science Foundation of China (U21B2092, 22202213, 22402210, 22502215, 22502214, 22572200, and 22579171)+3 种基金the International Partnership Program of Chinese Academy of Sciences (172GJHZ2022028MI)the Shenyang Bureau of Science and Technology (24-213-3-25)the Natural Science Foundation of Liaoning Province (2025BS0153)Zhongke Technology Achievement Transfer and Transformation Center of Henan Province 2025119
文摘Single-atom catalysts(SACs)have demonstrated excellent performance in heterogeneous catalytic reactions owing to their maximized atomic efficiency,distinctive geometric,and electronic configurations.However,the efficacy of SACs remains limited for certain reactions requiring simultaneous activation of multiple reactants over metallic active sites.Herein,we report an atomically dispersed Pt1Ru1 dual-atom pair site anchored on nanodiamond@graphene(ND@G)for CO oxidation.The Pt1Ru1 dual-atom catalyst shows an exceptional turnover frequency(TOF)of 17.6.10^(-2)s^(-1)at significantly lower temperature(30℃),achieving a tenfold increase in TOF compared to singleatom Pt1/ND@G catalyst(1.5.10^(-2)s^(-1))and surpassing to previously reported Pt-based catalysts under similar conditions.Moreover,the catalyst demonstrates excellent stability,maintaining its activity for 40 h at 80℃without significant deactivation.The superior catalytic performance of Pt-Ru dual-atom catalysts is attributed to the synergistic effect between Pt and Ru atoms with enhanced metallicity for improving simultaneous adsorption and activation of CO and O_(2),and the tuning of conventional competitive reactant adsorption into a non-competitive pathway over dual-atom pair sites.The present work manifests the advantages of dual-atom pair sites in heterogeneous catalysis and paves the way for precise design of catalysts at the atomic scale.
基金supported by National Research Foundation of Korea(NRF)funded by Ministry of Science and ICT(MSIT)(No.RS-2023-00260527,RS-2024-00407282,RS-2025-00557667)supported by Hanyang University Industry-University Cooperation Foundation(No.202400000003943)supported by Korea Planning&Evaluation Institute of Industrial Technology(KEIT)funded by South Korean Ministry of Trade,Industry and Energy(MOTIE)(No.RS-2025-25454815,RS-2025-02308064,20017382)。
文摘Oxide semiconductors(OSs),introduced by the Hosono group in the early 2000s,have evolved from display backplane materials to promising candidates for advanced memory and logic devices.The exceptionally low leakage current of OSs and compatibility with three-dimensional(3D)architectures have recently sparked renewed interest in their use in semiconductor applications.This review begins by exploring the unique material properties of OSs,which fundamentally originate from their distinct electronic band structure.Subsequently,we focus on atomic layer deposition(ALD),a core technique for growing excellent OS films,covering both basic and advanced processes compatible with 3D scaling.The basic surface reaction mechanisms—adsorption and reaction—and their roles in film growth are introduced.Furthermore,material design strategies,such as cation selection,crystallinity control,anion doping,and heterostructure engineering,are discussed.We also highlight challenges in memory applications,including contact resistance,hydrogen instability,and lack of p-type materials,and discuss the feasibility of ALD-grown OSs as potential solutions.Lastly,we provide an outlook on the role of ALD-grown OSs in memory technologies.This review bridges material fundamentals and device-level requirements,offering a comprehensive perspective on the potential of ALD-driven OSs for next-generation semiconductor memory devices.
基金supported by the Program for Guangdong Province Introduced Innovative and Entrepreneurial Team Program(2023ZT10L061)the NSFC Projects(Grant No.22402232)the Project supported by the Natural Science Foundation of Guangdong Province,China(Grant No.2025A1515011742).
文摘The development of atomically dispersed multi-metallic catalysts is imperative for tailoring catalytic performance and elucidating structure-activity relationships.However,synthesizing such precisely engineered architectures while maintaining atomic dispersion of distinct metal centers remains a formidable challenge due to thermodynamic instability and synthetic complexity.We herein propose a topological confinement pre-anchoring strategy via pre-anchoring spatially resolved Zn/Fe dual-metal sources in a structurally engineered metal-organic framework precursor to synthesize atomically dispersed ZnFe bimetallic single-atom catalysts.Extended X-ray absorption fine structure measurements and X-ray absorption near-edge structure reveal that the atomically dispersed Zn/Fe metal sites and electronic redistribution in ZnFe bimetallic single-atom catalysts.The ultrahigh surface area,hierarchical pore,and synergistic effect between Zn/Fe can greatly favor the exposure of the active site,mass transport,and improvement of intrinsic activity.Consequently,the ZnFe bimetallic single-atom catalyst demonstrates superior oxygen reduction reaction performance,achieving a half-wave potential of 0.86 V and delivering a kinetic current density of 10.1 mA cm^(-2)at 0.85 V versus RHE in 0.1 m KOH electrolyte.These metrics not only surpass those of commercial Pt/C,but also rival the highest-performing catalysts reported to date.The Zn-air battery built with ZnFe bimetallic single-atom catalyst exhibits high power density(278.5 mW cm^(-2))and specific discharging capacities(657 mAh g^(-1)).This work provides a new design pathway for constructing atomically dispersed multi-metal electrocatalysts for high-performance energy-related applications.
基金supported by the National Key Research and Development Program of China(Grant No.2023YFA1407001)the Department of Science and Technology of Jiangsu Province(Grant No.BK20220032)+1 种基金support from the Guang Dong Basic and Applied Basic Research Foundation(Grant No.2023A1515010365)support from the Postgraduate Research and Practice Innovation Program of Jiangsu Province under Grant No.KYCX25_1934。
文摘Heat dissipation highly relies on the thermal conductivity(κ)of materials.Materials with large bandgaps and signifcant atomic mass ratios,such as BAs,SiC,andθ-TaN,have attracted considerable attention due to their potential for achieving ultra-highκ,with BAs serving as a particularly representative example due to its unique combination of large bandgap and high thermal conductivity.In this paper,the efects of atomic mass modifcation on phonon bandgap andκare systematically investigated using a BAs model,accounting for both three-and four-phonon scattering processes.A 20%increase inκcan be obtained by substituting B,achieved through widening the phonon bandgap,which suppresses phonon scattering.Notably,the AAOO four-phonon scattering channel is more suppressed than the AAO three-phonon channel,leading to an increased phonon lifetime(τ).For As,κcan also be enhanced by 5%when replaced by lighter atoms,such as^(69)As,primarily due to the increased phonon group velocity(υ).We systematically clarify how atomic-mass-induced bandgap variations afectτ,υ,and thereforeκin wide-bandgap systems.Our work provides a specifc scheme for further improving the ultra-highκof materials with large bandgaps,which possesses great guiding signifcance.
基金supported by the Zhejiang Provincial Science and Technology Plan(“Jianbing and Lingyan”)project(Grant No.2024C01099)Beijing Natural Science Foundation-Non-Consensus Innovation Project(Grant No.F251046)+1 种基金National Natural Science Fund for Excellent Young Scientists Fund Program(Grant No.KZ37124001)the National Natural Science Foundation of China(Grant No.42388101).
文摘The powerful light field manipulation capability of metasurfaces offers a novel development perspective for the quantum precision measurement.By applying the phasegradient metasurface(PGM)to atomic magnetometers(AMs),we have proposed and experimentally demonstrated a new type of compact single-beam elliptically polarized atomic magnetometers(EPAMs).Employing the fabricated chiral beam splitter PGM with high cross-polarization transmittance,a new atomic spin chirality detection method was devised,enabling the ultra-high sensitivity for extremely weak magnetic field measurement and achieving a high sensitivity of 2.67 pT/Hz^(1/2)under an external magnetic field of approximately 10,000 nT.The new AMs combine the pumping and probing polarized light,achieving a compact design.The fabricated PGM has a size of only 3 mm×3 mm×0.7 mm,which is beneficial for the miniaturization and integration of AMs.This work effectively expands the application of metasurfaces in the field of quantum precision measurement,and also provides a new viewpoint for the design and development of high-sensitivity and miniaturized AMs.
基金supported by the National Natural Science Foundation of Chinathe Beijing Natural Science Foundationthe National Key R&D Program of China,and the Chinese Academy of Sciences.
文摘A research team led by Prof.YANG Kai at the Institute of Physics(IOP),Chinese Academy of Sciences,in collaboration with Prof.FERNÁNDEZ-ROSSIER Joaquín from International Iberian Nanotechnology Laboratory,has demonstrated all-electrical control of quantum interference in individual atomic spins on a surface,opening new possibilities for fast and robust quantum-state manipulation at the atomic scale.
文摘Single-atom catalysts (SACs) have emerged as a transformative class of materials in heterogeneous catalysis owing to their atomically dispersed metal centers, maximal atom utilization, and well-defined coordination environments. In the energy sector, SACs have shown exceptional performance in electrocatalytic reactions such as the oxygen reduction reaction (ORR), hydrogen evolution reaction (HER), and carbon dioxide reduction (CO_(2)RR), where their tunable local electronic structures facilitate high activity and selectivity under mild conditions. Meanwhile, in the environmental domain, SACs are increasingly explored for advanced oxidation processes (AOPs), particularly in water purification applications, due to their ability to generate reactive species from green oxidants like hydrogen peroxide or peroxymonosulfate (PMS). Among various AOP strategies, PMS-based Fenton-like reactions have gained attention due to the high oxidation potential and stability of PMS in a wide pH range.
基金supported by the National Key Research and Development Program of China(2022YFA1505700)National Natural Science Foundation of China(22475214 and 22205232)+2 种基金Talent Plan of Shanghai Branch,Chinese Academy of Sciences(CASSHB-QNPD-2023-020)Natural Science Foundation of Fujian Province(2023J06044)the Self-deployment Project Research Program of Haixi Institutes,Chinese Academy of Sciences(CXZX-2022-JQ06 and CXZX-2022-GH03)。
文摘Aberration-corrected annular dark-field scanning transmission electron microscopy(ADF-STEM)is a powerful tool for structural and chemical analysis of materials.Conventional analyses of ADF-STEM images rely on human labeling,making them labor-intensive and prone to subjective error.Here,we introduce a deep-learning-based workflow combining a pix2pix network for image denoising and either a mathematical algorithm local intensity threshold segmentation(LITS)or another deep learning network UNet for chemical identification.After denoising,the processed images exhibit a five-fold improvement in signal-to-noise ratio and a 20%increase in accuracy of atomic localization.Then,we take atomic-resolution images of Y–Ce dual-atom catalysts(DACs)and Fe-doped ReSe_(2) nanosheets as examples to validate the performance.Pix2pix is applied to identify atomic sites in Y–Ce DACs with a location recall of 0.88 and a location precision of 0.99.LITS is used to further differentiate Y and Ce sites by the intensity of atomic sites.Furthermore,pix2pix and UNet workflow with better automaticity is applied to identification of Fe-doped ReSe_(2) nanosheets.Three types of atomic sites(Re,the substitution of Fe for Re,and the adatom of Fe on Re)are distinguished with the identification recall of more than 0.90 and the precision of higher than 0.93.These results suggest that this strategy facilitates high-quality and automated chemical identification of atomic-resolution images.
文摘Single-atom Fe catalysts show significant promise in the electrocatalytic reduction of CO_(2)(CO_(2)RR),while their performance remains inferior to that of precious metal catalysts due to the overly strong binding of^(*)CO intermediates.Although the introduction of heteroatoms or transition metal sites can modulate the binding strength of^(*)CO on Fe sites,these regulators often induce competitive hydrogen evolution reaction(HER)with reduced Faraday efficiency(FE).In this work,we employ HER-inert Sn as a regulator to tune the electronic structure of Fe,weakening^(*)CO adsorption and enhancing CO_(2)RR performance.Diatomic Fe-Sn pairs supported on N-doped carbon(Fe-Sn/NC)were synthesized,achieving FE for CO exceeding 90%over a broad potential range from−0.4 to−0.9 V versus the reversible hydrogen electrode.Fe-Sn/NC shows a high turnover frequency of 1.5×10^(4)h^(-1),much higher than that of Fe/NC.Characterization results and theoretical calculations demonstrate that bonding Sn site to Fe generates electron-rich Fe centers,effectively reducing the adsorption strength of^(*)CO without triggering HER.Additionally,Fe-Sn/NC exhibits exceptional activity in hydrazine oxidation performance(HzOR).The HzOR-assisted CO_(2)RR system using Fe-Sn/NC as electrodes reduces energy consumption by 38%compared with the conventional CO_(2)RR coupled oxygen evolution reaction system.
基金supported by the Pre-research fund(No.412130024).
文摘The T_(1)(Al_(2) CuLi)phase is one of the most effective strengthening nanoscale-precipitate in Al-Cu alloys with Li.However,its formation and evolution still need to be further clarified during aging due to the complex precipitation sequences.Here,a detailed investigation has been carried out on the atomic struc-tural evolution of T_(1) precipitate in an aged Al-Cu-Li-Mg-Ag alloy using state-of-the-art Cs-corrected high-angle annular dark field(HAADF)-coupled with integrated differential phase contrast(iDPC)-scanning transmission electron microscopy(STEM)and energy-dispersive X-ray spectroscopy(EDXS)techniques.An intermediate T_(1)’phase between T_(1p) and T_(1) phase,with a crystal structure and orientation rela-tionship consistent with T_(1),but exhibiting different atomic occupancy and chemical composition was found.We observed the atomic structural transformation from T_(1p) to T_(1)’phase(fcc→hcp),involving only 1/12<112>Al shear component.DFT calculation results validated our proposed structural models and the precipitation sequence.Besides,the distributions of minor solute elements(Ag,Mg,and Zn)in the pre-cipitates exhibited significant differences.These findings may contribute to a further understanding of the nucleation mechanism of T_(1) precipitate.
基金financially supported by the Key Laboratory of Carbon-based Energy Molecular Chemical Utilization Technology in Guizhou Province(No.2023008)Guizhou Provincial Science and Technology Projects(No.ZKZD2023004)+1 种基金One Hundred Person Project of Guizhou Province(No.GCC 2023013)Scientific and Technological Innovation Talents Team Project of Guizhou Province(No.CXTD2023029).
文摘Metal-based catalysts are prevalent in the CO_(2) hydrogenation to methanol owing to their remarkable catalytic activity.Herein,Ru/In_(2)O_(3) catalysts with different morphologies obtained by doping Ru into In_(2)O_(3) with irregular,rod-like,and flower-like morphologies are used for catalytic CO_(2) hydrogenation to methanol.Results indicate that the flower-like Ru/In_(2)O_(3)(Ru/In_(2)O_(3)-F)exhibits higher catalytic performance than Ru/In_(2)O_(3) with other morphologies,achieving a 12.9%CO_(2) conversion,74.02%methanol selectivity,and 671.36 mg_(MeOH) h^(−1) g_(cat)^(−1) methanol spatiotemporal yield.Furthermore,Ru/In_(2)O_(3)-F maintains its catalytic stability over 200 h at 5 MPa and 290℃.The promotional effect mainly stems from the fact that electronic structure of Ru can be effectively adjusted by modulating the morphology of In_(2)O_(3).The strong interaction between atomically dispersed Ru and In_(2)O_(3)-F enhances the structural stability of Ru,inhibiting the agglomeration of the catalyst during the reaction process.Furthermore,density-functional theory calculations reveal that highly dispersed Ru atoms not only perform efficient and rapid electronic gain and loss processes,facilitating the catalytic activation of H_(2) into H intermediates.It also enables the generated reactive H to rapidly overflow to the surrounding In sites to participate in CO_(2) reduction.These findings provide a theoretical basis for the development of high-performance catalysts for CO_(2) hydrogenation.
基金financial support from the National Key Research and Development Program of China(2018YFA0703400)the Fundamental Research Funds for the Provincial Universities of Zhejiang(GK239909299001021)+1 种基金the Ninth China Association for Science and Technology Youth Talent Lift Project Support Plan(KYZ015324002)the Changjiang Scholars Program of Chinese Ministry of Education。
文摘Atomic surfaces are strictly required by high-performance devices of diamond.Nevertheless,diamond is the hardest material in nature,leading to the low material removal rate(MRR)and high surface roughness during machining.Noxious slurries are widely used in conventional chemical mechanical polishing(CMP),resulting in the possible pollution to the environment.Moreover,the traditional slurries normally contain more than four ingredients,causing difficulties to control the process and quality of CMP.To solve these challenges,a novel green CMP for single crystal diamond was developed,consisting of only hydrogen peroxide,diamond abrasive and Prussian blue(PB)/titania catalyst.After CMP,atomic surface is achieved with surface roughness Sa of 0.079 nm,and the MRR is 1168 nm·h^(-1).Thickness of damaged layer is merely 0.66 nm confirmed by transmission electron microscopy(TEM).X-ray photoelectron spectroscopy,electron paramagnetic resonance and TEM reveal that·OH radicals form under ultraviolet irradiation on PB/titania catalyst.The·OH radicals oxidize diamond,transforming it from monocrystalline to amorphous atomic structure,generating a soft amorphous layer.This contributes the high MRR and formation of atomic surface on diamond.The developed novel green CMP offers new insights to achieve atomic surface of diamond for potential use in their high-performance devices.
文摘Broadband transparent films play a pivotal role in various applications such as lenses and solar cells,particularly porous structured transparent films exhibit significant potential.This study investigates a porous SiO_(2) refractive index gradient anti-reflective film prepared by atomic layer deposition(ALD).A porous SiO_(2) film with gradual porosity was obtained by phosphoric acid etching of Al_(2)O_(3)/SiO_(2) multilayers with gradient Al2O3 ratios,achieving a gradual decrease in refractive index from the substrate to the surface.The film exhibited an average transmittance as high as 97.8%within the wavelength range from 320 nm to 1200 nm.The environmental adaptability was further enhanced by surface modification using rare earth oxide(REO)La_(2)O_(3),resulting in formation of a lotus leaf-like structure and achieving a water contact angle of 100.0°.These data proved that the modification significantly improved hydrophobic self-cleaning capability while maintaining exceptional transparency of the film.The surface structure of the modified film remained undamaged even after undergoing wipe testing,demonstrating its excellent surface durability.
