Simple power analysis is the most devastating attack on the security of elliptic curve scalar multiplication and can probably retrieve the secret key. In this paper,we analyze the formulas of point doubling and additi...Simple power analysis is the most devastating attack on the security of elliptic curve scalar multiplication and can probably retrieve the secret key. In this paper,we analyze the formulas of point doubling and addition on Jacobi-quartic Curve in projective coordination. In addition,a fast and secure side-channel atomic scalar multiplication algorithm is proposed using the side-channel atomic block. Compared with the previous methods,the new algorithm is more efficient. For 192 bits scalar using NAF recoding,the efficiency of the new algorithm is increased by about 6.7%～23% if S/M=0.8 or 12.7%～33.2% if S/M=0.6.展开更多
Platinum clusters(Pt_(n))are extensively used as electrocatalysts for oxygen reduction reaction(ORR)because they provide excellent performance together with a reduced Pt requirement.However,the precise synthesis and a...Platinum clusters(Pt_(n))are extensively used as electrocatalysts for oxygen reduction reaction(ORR)because they provide excellent performance together with a reduced Pt requirement.However,the precise synthesis and atomic-level insights into the structure-activity relationship of Pt_(n) remain a great challenge.Here,we present a combinatorial synthesis and analysis method to investigate the atomicity-activity relationships of Pt_(n) at the individual level.We employ single nanoparticle collision electrochemistry to facilitate the in-situ electrodeposition of a single precisely tunable Pt_(n) on the graphene quantum dot support,followed by instantaneous measurement of the intrinsic ORR activity of the resulting Pt_(n).By relying on highly sensitive electrochemical measurements,our investigations clarify the atomicity-specific ORR activity of Pt_(n),which is attributed to their distinct geometric and electronic structures at varying cluster sizes.Significantly,Pt_(n) with low atomicity,especially below 20,can reach extraordinarily high ORR activities due to atom-by-atom arrangement.Our work provides a simple and efficient method for investigating the atomicity-activity relationships of other nanoclusters under real reaction conditions,enabling a better design of the electrocatalysts at the atomic level.展开更多
In this article,we conduct a study on mixed quasi-martingale Hardy spaces that are defined by means of the mixed L_(p)-norm.By utilizing Doob’s inequalities,we explore the atomic decomposition and quasi-martingale in...In this article,we conduct a study on mixed quasi-martingale Hardy spaces that are defined by means of the mixed L_(p)-norm.By utilizing Doob’s inequalities,we explore the atomic decomposition and quasi-martingale inequalities of mixed quasi-martingale Hardy spaces.Moreover,we furnish sufficient conditions for the boundedness ofσ-sublinear operators in these spaces.These findings extend the existing conclusions regarding mixed quasi-martingale Hardy spaces defined with the help of the mixed L_(p)-norm.展开更多
Scalability remains a major challenge in building practical fault-tolerant quantum computers.Currently,the largest number of qubits achieved across leading quantum platforms ranges from hundreds to thousands.In atom a...Scalability remains a major challenge in building practical fault-tolerant quantum computers.Currently,the largest number of qubits achieved across leading quantum platforms ranges from hundreds to thousands.In atom arrays,scalability is primarily constrained by the capacity to generate large numbers of optical tweezers,and conventional techniques using acousto-optic deflectors or spatial light modulators struggle to produce arrays much beyond∼10,000 tweezers.Moreover,these methods require additional microscope objectives to focus the light into micrometer-sized spots,which further complicates system integration and scalability.Here,we demonstrate the experimental generation of an optical tweezer array containing 280×280 spots using a metasurface,nearly an order of magnitude more than most existing systems.The metasurface leverages a large number of subwavelength phase-control pixels to engineer the wavefront of the incident light,enabling both large-scale tweezer generation and direct focusing into micron-scale spots without the need for a microscope.This result shifts the scalability bottleneck for atom arrays from the tweezer generation hardware to the available laser power.Furthermore,the array shows excellent intensity uniformity exceeding 90%,making it suitable for homogeneous single-atom loading and paving the way for trapping arrays of more than 10,000 atoms in the near future.展开更多
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
We prepared Co_(x)Pt_(100-x)(x=40,45,50,55,60)nanoparticles by the sol-gel method.The phase composition and crystal structure,morphology and microstructure,and magnetic properties of the samples were characterized and...We prepared Co_(x)Pt_(100-x)(x=40,45,50,55,60)nanoparticles by the sol-gel method.The phase composition and crystal structure,morphology and microstructure,and magnetic properties of the samples were characterized and tested using X-ray diffraction(XRD),transmission electron microscopy(TEM),and vibrating sample magnetometer(VSM),respectively.The results demonstrate that the coercivity of CoPt nanoparticles can be effectively controlled by adjusting the atomic ratio of Co and Pt in the samples.Among the compositions studied,the Co_(45)Pt_(55)sample synthesized by the sol-gel method exhibits smaller grain size and a coercivity as high as 6.65×10^(5) A/m is achieved.The morphology and microstructure of the nanoparticles were analyzed by TEM images,indicating that a slight excess of Pt can effectively enhance the coercivity of CoPt nanoparticles.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
The development of catalytic multicomponent reactions for constructing complex organic scaffolds from readily accessible commodity chemicals is a key pursuit in contemporary synthetic chemistry.Current methods for syn...The development of catalytic multicomponent reactions for constructing complex organic scaffolds from readily accessible commodity chemicals is a key pursuit in contemporary synthetic chemistry.Current methods for synthesizing thioesters primarily rely on the acylation of thiols,which produces substantial waste and requires malodorous,unstable sulfur sources.In this work,we introduce a photocatalyzed hydrogen transfer strategy that enables a three-component synthesis of thioesters using abundant primary alcohols,easily available alkenes and elemental sulfur under mild conditions.This protocol demonstrates broad applicability and high chemo-and regioselectivity for both primary alcohols and alkenes,highlighting the advantage and potential of photo-mediated hydrogen transfer in facilitating multicomponent reactions using primary alcohol and elemental sulfur feedstocks.展开更多
The development of catalysts with highly efficient oxygen evolution performance and low-Ir loading is key to scaling up the application of proton exchange membrane(PEM)water electrolysis technology.Here,an Ir-skin cat...The development of catalysts with highly efficient oxygen evolution performance and low-Ir loading is key to scaling up the application of proton exchange membrane(PEM)water electrolysis technology.Here,an Ir-skin catalyst(Ir@KM)is realized on a potassium-manganese oxide(K_(0.25)MnO_(x)(KM))using an ion-exchange method.The Ir-skin over the prepared Ir@KM has a low Ir-Ir atomic distance,endowing an energetically favorable oxide path mechanism to allow a low theoretical overpotential of 0.13 V.Ir@KM offers a low overpotential of~280 mV at a current density of 10 mA cm^(-2)and provides a high mass activity of up to 18,500 A at a cell voltage of 1.8 V in PEM,which is 17.6 times higher than that of IrO_(2),demonstrating a significant advantage in reducing the cost of the membrane electrode.The presented Ir-skin concept represents a promising strategy to fabricate low-Ir catalyst with high activity and durability for practical applications of PEM.展开更多
Ice premelting,the formation of a quasi-liquid layer on ice surfaces below the bulk melting point,plays a crucial role in various processes,ranging from glacier dynamics to ice friction and surface chemistry.Despite i...Ice premelting,the formation of a quasi-liquid layer on ice surfaces below the bulk melting point,plays a crucial role in various processes,ranging from glacier dynamics to ice friction and surface chemistry.Despite intensive research,the microscopic structure of the premelting layer and underlying molecular mechanisms remain poorly understood.In this work,we studied the temperature-and pressure-dependent structural disordering of crystalline Ih(0001)surface near the onset of premelting on the atomic scale by qPlus-based cryogenic atomic force microscopy.The linear correlation between the density of planar local structure(PLS)and the fraction of disordered surface region showed that the PLS mediated early-stage premelting by serving as a metastable seeding state.Notably,the associated surface disordering is cooperative,extending over an area of roughly~2 nm^(2) around a PLS.We further found a striking structural similarity between the kinetic-trapped regime below the surface crystallization temperature(T_(c))and the premelting-dominated regime above T_(c).As the deposition pressure increased,the characteristic temperature dependence was preserved,with only T_(c) shifting to higher values due to kinetic effects.Finally,we proposed a surface phase diagram for ice Ih(0001)based on our experimental observations.展开更多
Fenton-like technology based on peroxymonosulfate activation has shown great potential in refractory organics degradation.In this work,single Fe atom catalysts were synthesized through facile ball milling and exhibite...Fenton-like technology based on peroxymonosulfate activation has shown great potential in refractory organics degradation.In this work,single Fe atom catalysts were synthesized through facile ball milling and exhibited very high performance in peroxymonosulfate activation.The Fe single-atom filled an N vacancy on the triazine ring edge of C_(3)N_(4),as confirmed through X-ray absorption fine structure,density functional calculation and elec-tron paramagnetic resonance.The SAFe_(0.4)–C_(3)N_(4)/PMS system could completely remove phenol(20 mg/L)within 10 min and its first-order kinetic constant was 12.3 times that of the Fe_(3)O_(4)/PMS system.Under different ini-tial pH levels and in various anionic environments,SAFe_(0.4)–C_(3)N_(4) still demonstrated excellent catalytic activity,achieving a removal rate of over 90%for phenol within 12 min.In addition,SAFe_(0.4)–C_(3)N_(4) exhibited outstanding selectivity in reaction systems with different pollutants,showing excellent degradation effects on electron-rich pollutants only.Hydroxyl radicals(•OH),singlet oxygen(1O_(2))and high-valent iron oxide(Fe(Ⅳ)=O)were de-tected in the SAFe_(0.4)–C_(3)N_(4)/PMS system through free radical capture experiments.Further experiments on the quenching of active species and a methyl phenyl sulfoxide probe confirmed that 1O_(2) and Fe(Ⅳ)=O played dom-inant roles.Additionally,the change in the current response after adding PMS and phenol in succession proved that a direct electron transfer path between organic matter and the catalyst surface was unlikely to exist in the SAFe_(0.4)–C_(3)N_(4)/PMS/Phenol degradation system.This study provides a new demonstration of the catalytic mech-anism of single-atom catalysts.展开更多
The dissolvable polysulfides and sluggish Li_2S conversion kinetics are acknowledged as two significant challenges in the application lithium-sulfur(Li-S)batteries.Herein,we introduce a dual-doping strategy to modulat...The dissolvable polysulfides and sluggish Li_2S conversion kinetics are acknowledged as two significant challenges in the application lithium-sulfur(Li-S)batteries.Herein,we introduce a dual-doping strategy to modulate the electronic structure of MoS_(2),thereby obtaining a multifunctional catalyst that serves as an efficient sulfur host.The W/V dual single-atomdoped MoS_(2)grown on carbon nanofibers(CMWVS)demonstrates a strong adsorption ability for lithium polysulfides,suppressing the shuttle effects.Additionally,the doping process also results in the phase transition from 2H-MoS_(2)to 1T-MoS_(2)and generates sufficient edge sulfur atoms,promoting the charge/electron transfer and enriching the reaction sites.All these merits contribute to the superior conversion reaction kinetics,leading to the outstanding Li-S battery performance.When fabricated as cathodes by compositing with sulfur,the CMWVS/S cathode delivers a high capacity of 1481.7 mAh g^(-1)at 0.1 C(1 C=1672 mAh g^(-1))and maintains 816.3 m Ah g^(-1)after 1000 cycles at 1.0 C,indicating outstanding cycling stability.Even under a high sulfur loading of 7.9 mg cm^(-2)and lean electrolyte conditions(E/S ratio of 9.0μL mg^(-1)),the cathode achieves a high areal capacity of 8.2 m Ah cm^(-2),showing great promise for practical Li-S battery applications.This work broadens the scope of doping strategies in transition-metal dichalcogenides by tailoring their electronic structures,providing insightful direction for the rational development of high-efficiency electrocatalysts for advanced Li-S battery applications.展开更多
A visible-light-induced synergistic hydrogen atom transfer(HAT)and proton transfer(PT)catalysis was developed for the defluorinative carboxylation of α-CF_(2)R-substituted alkenes.This system affords a variety of γ,...A visible-light-induced synergistic hydrogen atom transfer(HAT)and proton transfer(PT)catalysis was developed for the defluorinative carboxylation of α-CF_(2)R-substituted alkenes.This system affords a variety of γ,γ-difluoro-and γ-monofluoro-vinylacetic acids without stepwise acidification,exhibiting good functional group tolerance,broad scope,and facile scalability.Mechanism studies support that thiol plays the role of the hydrogen relay,which s a hydrogen atom through HAT and then outputs a proton via PT.This strategy also takes full advantage of formate for photocatalytic carboxylation reaction in a step-and atomeconomical way.展开更多
Metal-support interaction(MSI) is crucial for fine-tuning the active-site structure of supported catalysts and enhancing performance.Here,we present an ammonia-directed reactive gas-metal-support interaction(RGMSI),in...Metal-support interaction(MSI) is crucial for fine-tuning the active-site structure of supported catalysts and enhancing performance.Here,we present an ammonia-directed reactive gas-metal-support interaction(RGMSI),in which NH_(3) reduces ZnO and assembles an anti-perovskite Ni_(3)ZnN structure with interstitial nitrogen,significantly boosting hydrogenation efficiency.Nitrogen incorporation expands the lattice parameter,increasing the(111) lattice spacing from 2.04Å in Ni to 2.18Å in Ni_(3)ZnN,with an extended Ni-Ni interatomic distance from 2.49Å to 2.65Å.Additionally,Ni-N coordination shifts the d-band center downward and induces electron deficiency in Ni via charge transfer.These modifications optimize reactant adsorption on the tailored Ni_(3)ZnN structure compared to Ni,leading to a remarkable increase in 1,3-butadiene hydrogenation selectivity from 30.0 % to 92.9 %,along with an enhanced TOF from 0.067 s^(-1) to 0.079 s^(-1).These findings highlight RGMSI as a versatile and effective strategy for designing supported metal catalysts,offering new insights into selective hydrogenation catalysis.展开更多
High-pressure electrides,characterized by the presence of interstitial quasi-atoms(ISQs),possess unique electronic structures and physical properties,such as diverse dimensions of electride states exhibiting different...High-pressure electrides,characterized by the presence of interstitial quasi-atoms(ISQs),possess unique electronic structures and physical properties,such as diverse dimensions of electride states exhibiting different superconductivity,which has attracted significant attention.Here,we report a new electron-deficient type of electride Li_(4)Al and identify its phase transition progress with pressurization,where the internal driving force behind phase transitions,bonding characteristics,and superconducting behaviors have been revealed based on first-principles density functional theory.Through analysis of the bonding properties of electride Li_(4)Al,we demonstrate that the ISQs exhibiting increasingly covalent characteristics between Al ions play a critical role in driving the phase transition.Our electron–phonon coupling calculations indicate that all phases exhibit superconducting behaviors.Importantly,we prove that the ISQs behave as free electrons and demonstrate that the factor governing T_(c) is primarily derived from Li-p-hybridized electronic states with ISQ compositions.These electronic states are scattered by low-frequency phonons arising from mixed vibrations of Li and Al affected by ISQs to enhance electron–phonon coupling.Our study largely expands the research scope of electrides,provides new insight for understanding phase transitions,and elucidates the effects of ISQs on superconducting behavior.展开更多
We report the results of the experiment on synthesizing ^(287,288)Mc isotopes (Z=115) using the fusionevaporation reaction ^(243)Am(^(48)Ca,4n,3n)^(287,288)Mc at the Spectrometer for Heavy Atoms and Nuclear Structure-...We report the results of the experiment on synthesizing ^(287,288)Mc isotopes (Z=115) using the fusionevaporation reaction ^(243)Am(^(48)Ca,4n,3n)^(287,288)Mc at the Spectrometer for Heavy Atoms and Nuclear Structure-2(SHANS2),a gas-filled recoil separator located at the China Accelerator Facility for Superheavy Elements(CAFE2).In total,20 decay chains are attributed to ^(288)Mc and 1 decay chain is assigned to ^(287)Mc.The measured oa-decay properties of ^(287,288)Mc as well as its descendants are consistent with the known data.No additional decay chains originating from the 2n or 5n reaction channels were detected.The excitation function of the ^(243)Am(^(48)Ca,3n)^(288)Mc reaction was measured at the cross-section level of picobarn,which indicates the promising capability for the study of heavy and superheavy nuclei at the facility.展开更多
This paper presents the high-order nonlinear spectrum of six-wave mixing(SWM)influenced by ionizing Rydberg atom environment in rubidium thermal vapor.The experimentally measured transmitted SWM signals reveal signifi...This paper presents the high-order nonlinear spectrum of six-wave mixing(SWM)influenced by ionizing Rydberg atom environment in rubidium thermal vapor.The experimentally measured transmitted SWM signals reveal significant spectrum shifts and novel regularities,providing nonlinear spectrum insights into the ionization characteristics of Rydberg atoms.The detailed spectrum variations with increasing ion density are presented,paving the way for multi-wave mixing distribution of plasma and demonstrating SWM’s potential as a tool for measuring the electric field induced by the ionization process.展开更多
350 keV He^(+) ions were injected into laser powder bed fusion(LPBF)-processed 304L stainless steel and traditional rolled 304L stainless steel with a flux of 1×10^(17) ions/cm^(2) at room temperature,followed by...350 keV He^(+) ions were injected into laser powder bed fusion(LPBF)-processed 304L stainless steel and traditional rolled 304L stainless steel with a flux of 1×10^(17) ions/cm^(2) at room temperature,followed by annealing at 750℃ for 10,100,and 300 h,respectively.The results showed that material swelling due to helium bubble coarsening was almost not observed in either the LPBF or rolled samples after 10 h of annealing duration.Rapid coarsening and swelling of bubbles occurred in the rolled samples,but only moderate bubble growth occurred in the LPBF sample after annealing for 100 h.After annealing for 300 h,the helium bubbles in both samples tended to grow steadily.For 10 h of annealing,the irradiated samples were in a disequilibrium state,and the apparent activation energy(E^(act))calculated by the Arrhenius model determined that helium atoms tended to diffuse through the displacement mechanism,and helium bubbles grew under the migration and coalescence(MC)mechanism.With annealing times over 100 h,the high-density dislocations and nano-oxide particles in the LPBF sample still had a strong trapping effect on the movement and growth of helium bubbles.After annealing for 300 h,the cellular subgrains in the LPBF sample decomposed,and the nano-oxide particles had no trapping effect on the helium bubbles.At this time,the dislocation structure played a primary role in suppressing the growth of helium bubbles,and the radiation resistance of the LPBF sample remained superior to that of the rolled samples.展开更多
基金sponsored and financial supported by National Natural Science Foundation of China (NSFC), grant No.61003121Sichuan Province High Technology Program under No.2009CD00014
文摘Simple power analysis is the most devastating attack on the security of elliptic curve scalar multiplication and can probably retrieve the secret key. In this paper,we analyze the formulas of point doubling and addition on Jacobi-quartic Curve in projective coordination. In addition,a fast and secure side-channel atomic scalar multiplication algorithm is proposed using the side-channel atomic block. Compared with the previous methods,the new algorithm is more efficient. For 192 bits scalar using NAF recoding,the efficiency of the new algorithm is increased by about 6.7%～23% if S/M=0.8 or 12.7%～33.2% if S/M=0.6.
基金financially supported by the National Natural Science Foundation of China(22272052)the Major Research Project(92061108)the Science and Technology Commission of Shanghai Municipality(24DX1400200)。
文摘Platinum clusters(Pt_(n))are extensively used as electrocatalysts for oxygen reduction reaction(ORR)because they provide excellent performance together with a reduced Pt requirement.However,the precise synthesis and atomic-level insights into the structure-activity relationship of Pt_(n) remain a great challenge.Here,we present a combinatorial synthesis and analysis method to investigate the atomicity-activity relationships of Pt_(n) at the individual level.We employ single nanoparticle collision electrochemistry to facilitate the in-situ electrodeposition of a single precisely tunable Pt_(n) on the graphene quantum dot support,followed by instantaneous measurement of the intrinsic ORR activity of the resulting Pt_(n).By relying on highly sensitive electrochemical measurements,our investigations clarify the atomicity-specific ORR activity of Pt_(n),which is attributed to their distinct geometric and electronic structures at varying cluster sizes.Significantly,Pt_(n) with low atomicity,especially below 20,can reach extraordinarily high ORR activities due to atom-by-atom arrangement.Our work provides a simple and efficient method for investigating the atomicity-activity relationships of other nanoclusters under real reaction conditions,enabling a better design of the electrocatalysts at the atomic level.
基金Supported by the National Natural Science Foundation of China(11871195)。
文摘In this article,we conduct a study on mixed quasi-martingale Hardy spaces that are defined by means of the mixed L_(p)-norm.By utilizing Doob’s inequalities,we explore the atomic decomposition and quasi-martingale inequalities of mixed quasi-martingale Hardy spaces.Moreover,we furnish sufficient conditions for the boundedness ofσ-sublinear operators in these spaces.These findings extend the existing conclusions regarding mixed quasi-martingale Hardy spaces defined with the help of the mixed L_(p)-norm.
基金supported by the National Natural Science Foundation of China (Grant No.92576208)Tsinghua University Initiative Scientific Research Program+1 种基金Beijing Science and Technology Planning ProjectTsinghua University Dushi Program。
文摘Scalability remains a major challenge in building practical fault-tolerant quantum computers.Currently,the largest number of qubits achieved across leading quantum platforms ranges from hundreds to thousands.In atom arrays,scalability is primarily constrained by the capacity to generate large numbers of optical tweezers,and conventional techniques using acousto-optic deflectors or spatial light modulators struggle to produce arrays much beyond∼10,000 tweezers.Moreover,these methods require additional microscope objectives to focus the light into micrometer-sized spots,which further complicates system integration and scalability.Here,we demonstrate the experimental generation of an optical tweezer array containing 280×280 spots using a metasurface,nearly an order of magnitude more than most existing systems.The metasurface leverages a large number of subwavelength phase-control pixels to engineer the wavefront of the incident light,enabling both large-scale tweezer generation and direct focusing into micron-scale spots without the need for a microscope.This result shifts the scalability bottleneck for atom arrays from the tweezer generation hardware to the available laser power.Furthermore,the array shows excellent intensity uniformity exceeding 90%,making it suitable for homogeneous single-atom loading and paving the way for trapping arrays of more than 10,000 atoms in the near future.
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Funded by the National Natural Science Foundation of China(No.52371169)。
文摘We prepared Co_(x)Pt_(100-x)(x=40,45,50,55,60)nanoparticles by the sol-gel method.The phase composition and crystal structure,morphology and microstructure,and magnetic properties of the samples were characterized and tested using X-ray diffraction(XRD),transmission electron microscopy(TEM),and vibrating sample magnetometer(VSM),respectively.The results demonstrate that the coercivity of CoPt nanoparticles can be effectively controlled by adjusting the atomic ratio of Co and Pt in the samples.Among the compositions studied,the Co_(45)Pt_(55)sample synthesized by the sol-gel method exhibits smaller grain size and a coercivity as high as 6.65×10^(5) A/m is achieved.The morphology and microstructure of the nanoparticles were analyzed by TEM images,indicating that a slight excess of Pt can effectively enhance the coercivity of CoPt nanoparticles.
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)+4 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 2025119The XAS experiments were conducted in Beijing Synchrotron Radiation Facility(BSRF)and Shanghai Synchrotron Radiation Facility(SSRF).
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National Natural Science Foundation of China (Nos.22071185 and 22271224)the Fundamental Research Funds for the Central Universities (No.2042019kf0008)Wuhan University startup funding for financial support。
文摘The development of catalytic multicomponent reactions for constructing complex organic scaffolds from readily accessible commodity chemicals is a key pursuit in contemporary synthetic chemistry.Current methods for synthesizing thioesters primarily rely on the acylation of thiols,which produces substantial waste and requires malodorous,unstable sulfur sources.In this work,we introduce a photocatalyzed hydrogen transfer strategy that enables a three-component synthesis of thioesters using abundant primary alcohols,easily available alkenes and elemental sulfur under mild conditions.This protocol demonstrates broad applicability and high chemo-and regioselectivity for both primary alcohols and alkenes,highlighting the advantage and potential of photo-mediated hydrogen transfer in facilitating multicomponent reactions using primary alcohol and elemental sulfur feedstocks.
基金supported by the Hainan Province Science and Technology Special Fund(ZDYF2023GXJS165)the National Natural Science Foundation of China(52164028,22109035,52274297)+2 种基金the Foundation of State Key Laboratory of Marine Resource Utilization in South China Sea(Hainan University,MRUKF2021029)the Start-up Research Foundation of Hainan University(KYQD(ZR)-20008,20084,21170)the Specific Research Fund of the Innovation Platform for Academicians of Hainan Province。
文摘The development of catalysts with highly efficient oxygen evolution performance and low-Ir loading is key to scaling up the application of proton exchange membrane(PEM)water electrolysis technology.Here,an Ir-skin catalyst(Ir@KM)is realized on a potassium-manganese oxide(K_(0.25)MnO_(x)(KM))using an ion-exchange method.The Ir-skin over the prepared Ir@KM has a low Ir-Ir atomic distance,endowing an energetically favorable oxide path mechanism to allow a low theoretical overpotential of 0.13 V.Ir@KM offers a low overpotential of~280 mV at a current density of 10 mA cm^(-2)and provides a high mass activity of up to 18,500 A at a cell voltage of 1.8 V in PEM,which is 17.6 times higher than that of IrO_(2),demonstrating a significant advantage in reducing the cost of the membrane electrode.The presented Ir-skin concept represents a promising strategy to fabricate low-Ir catalyst with high activity and durability for practical applications of PEM.
基金Project supported by the National Key R&D Program of China(Grant Nos.2021YFA1400500 and 2025YFF1502400)the National Natural Science Foundation of China(Grant Nos.92361302,12250001,12535001,and U22A20260)+3 种基金the China Postdoctoral Science Foundation(Grant Nos.BX20230021,2023T160011,and 2024M760068)support from the National Program for Support of Top-notch Young professionalssupport from Beijing Outstanding Young Scientist Program(Grant No.JWZQ20240101002)the New Cornerstone Science Foundation through the New Cornerstone Investigator Program and the XPLORER PRIZE。
文摘Ice premelting,the formation of a quasi-liquid layer on ice surfaces below the bulk melting point,plays a crucial role in various processes,ranging from glacier dynamics to ice friction and surface chemistry.Despite intensive research,the microscopic structure of the premelting layer and underlying molecular mechanisms remain poorly understood.In this work,we studied the temperature-and pressure-dependent structural disordering of crystalline Ih(0001)surface near the onset of premelting on the atomic scale by qPlus-based cryogenic atomic force microscopy.The linear correlation between the density of planar local structure(PLS)and the fraction of disordered surface region showed that the PLS mediated early-stage premelting by serving as a metastable seeding state.Notably,the associated surface disordering is cooperative,extending over an area of roughly~2 nm^(2) around a PLS.We further found a striking structural similarity between the kinetic-trapped regime below the surface crystallization temperature(T_(c))and the premelting-dominated regime above T_(c).As the deposition pressure increased,the characteristic temperature dependence was preserved,with only T_(c) shifting to higher values due to kinetic effects.Finally,we proposed a surface phase diagram for ice Ih(0001)based on our experimental observations.
基金supported by the National Natural Science Foundation of China(Nos.22406081,22276086,22306086)the Natural Science Foundation of Jiangxi Province(No.20232BAB213029),all of which are greatly acknowledged by the authors.
文摘Fenton-like technology based on peroxymonosulfate activation has shown great potential in refractory organics degradation.In this work,single Fe atom catalysts were synthesized through facile ball milling and exhibited very high performance in peroxymonosulfate activation.The Fe single-atom filled an N vacancy on the triazine ring edge of C_(3)N_(4),as confirmed through X-ray absorption fine structure,density functional calculation and elec-tron paramagnetic resonance.The SAFe_(0.4)–C_(3)N_(4)/PMS system could completely remove phenol(20 mg/L)within 10 min and its first-order kinetic constant was 12.3 times that of the Fe_(3)O_(4)/PMS system.Under different ini-tial pH levels and in various anionic environments,SAFe_(0.4)–C_(3)N_(4) still demonstrated excellent catalytic activity,achieving a removal rate of over 90%for phenol within 12 min.In addition,SAFe_(0.4)–C_(3)N_(4) exhibited outstanding selectivity in reaction systems with different pollutants,showing excellent degradation effects on electron-rich pollutants only.Hydroxyl radicals(•OH),singlet oxygen(1O_(2))and high-valent iron oxide(Fe(Ⅳ)=O)were de-tected in the SAFe_(0.4)–C_(3)N_(4)/PMS system through free radical capture experiments.Further experiments on the quenching of active species and a methyl phenyl sulfoxide probe confirmed that 1O_(2) and Fe(Ⅳ)=O played dom-inant roles.Additionally,the change in the current response after adding PMS and phenol in succession proved that a direct electron transfer path between organic matter and the catalyst surface was unlikely to exist in the SAFe_(0.4)–C_(3)N_(4)/PMS/Phenol degradation system.This study provides a new demonstration of the catalytic mech-anism of single-atom catalysts.
基金supported by the National Natural Science Foundation of China(52402166)the Science and Technology Development Fund+2 种基金Macao SAR(0065/2023/AFJ,0116/2022/A3)the Australian Research Council(DE220100154)the Natural Science Foundation of Guangdong Province(2025A1515011120)。
文摘The dissolvable polysulfides and sluggish Li_2S conversion kinetics are acknowledged as two significant challenges in the application lithium-sulfur(Li-S)batteries.Herein,we introduce a dual-doping strategy to modulate the electronic structure of MoS_(2),thereby obtaining a multifunctional catalyst that serves as an efficient sulfur host.The W/V dual single-atomdoped MoS_(2)grown on carbon nanofibers(CMWVS)demonstrates a strong adsorption ability for lithium polysulfides,suppressing the shuttle effects.Additionally,the doping process also results in the phase transition from 2H-MoS_(2)to 1T-MoS_(2)and generates sufficient edge sulfur atoms,promoting the charge/electron transfer and enriching the reaction sites.All these merits contribute to the superior conversion reaction kinetics,leading to the outstanding Li-S battery performance.When fabricated as cathodes by compositing with sulfur,the CMWVS/S cathode delivers a high capacity of 1481.7 mAh g^(-1)at 0.1 C(1 C=1672 mAh g^(-1))and maintains 816.3 m Ah g^(-1)after 1000 cycles at 1.0 C,indicating outstanding cycling stability.Even under a high sulfur loading of 7.9 mg cm^(-2)and lean electrolyte conditions(E/S ratio of 9.0μL mg^(-1)),the cathode achieves a high areal capacity of 8.2 m Ah cm^(-2),showing great promise for practical Li-S battery applications.This work broadens the scope of doping strategies in transition-metal dichalcogenides by tailoring their electronic structures,providing insightful direction for the rational development of high-efficiency electrocatalysts for advanced Li-S battery applications.
基金supported by the National Natural Science Foundation of China (22472031,U24A20567,22032002)the 111 Project。
文摘A visible-light-induced synergistic hydrogen atom transfer(HAT)and proton transfer(PT)catalysis was developed for the defluorinative carboxylation of α-CF_(2)R-substituted alkenes.This system affords a variety of γ,γ-difluoro-and γ-monofluoro-vinylacetic acids without stepwise acidification,exhibiting good functional group tolerance,broad scope,and facile scalability.Mechanism studies support that thiol plays the role of the hydrogen relay,which s a hydrogen atom through HAT and then outputs a proton via PT.This strategy also takes full advantage of formate for photocatalytic carboxylation reaction in a step-and atomeconomical way.
基金the financial support provided by the National Natural Science Foundation of China (Nos.22072164,22472180,22002173)Energy Revolution S&T Program of Yulin Innovation Institute of Clean Energy (No.E411030705)+2 种基金Natural Science Foundation of Liaoning Province (No.2022-MS004)China Postdoctoral Science Foundation (No.2020M680999)the Research Fund of Shenyang National Laboratory for Materials Science。
文摘Metal-support interaction(MSI) is crucial for fine-tuning the active-site structure of supported catalysts and enhancing performance.Here,we present an ammonia-directed reactive gas-metal-support interaction(RGMSI),in which NH_(3) reduces ZnO and assembles an anti-perovskite Ni_(3)ZnN structure with interstitial nitrogen,significantly boosting hydrogenation efficiency.Nitrogen incorporation expands the lattice parameter,increasing the(111) lattice spacing from 2.04Å in Ni to 2.18Å in Ni_(3)ZnN,with an extended Ni-Ni interatomic distance from 2.49Å to 2.65Å.Additionally,Ni-N coordination shifts the d-band center downward and induces electron deficiency in Ni via charge transfer.These modifications optimize reactant adsorption on the tailored Ni_(3)ZnN structure compared to Ni,leading to a remarkable increase in 1,3-butadiene hydrogenation selectivity from 30.0 % to 92.9 %,along with an enhanced TOF from 0.067 s^(-1) to 0.079 s^(-1).These findings highlight RGMSI as a versatile and effective strategy for designing supported metal catalysts,offering new insights into selective hydrogenation catalysis.
基金supported by the National Key Research and Development Program of China (Grant Nos.2023YFA1406200 and 2022YFA-1405500)the National Natural Science Foundation of China (Grant Nos.12304021 and 52072188)+3 种基金Zhejiang Provincial Natural Science Foundation of China (Grant Nos.LQ23A040004 and MS26A040028)Natural Science Foundation of Ningbo (Grant Nos.2022J091 and ZX2025001430)the Program for Science and Technology Innovation Team in Zhejiang (Grant No.2021R01004)the Program for Changjiang Scholars and Innovative Research Team in University (Grant No.IRT_15R23)。
文摘High-pressure electrides,characterized by the presence of interstitial quasi-atoms(ISQs),possess unique electronic structures and physical properties,such as diverse dimensions of electride states exhibiting different superconductivity,which has attracted significant attention.Here,we report a new electron-deficient type of electride Li_(4)Al and identify its phase transition progress with pressurization,where the internal driving force behind phase transitions,bonding characteristics,and superconducting behaviors have been revealed based on first-principles density functional theory.Through analysis of the bonding properties of electride Li_(4)Al,we demonstrate that the ISQs exhibiting increasingly covalent characteristics between Al ions play a critical role in driving the phase transition.Our electron–phonon coupling calculations indicate that all phases exhibit superconducting behaviors.Importantly,we prove that the ISQs behave as free electrons and demonstrate that the factor governing T_(c) is primarily derived from Li-p-hybridized electronic states with ISQ compositions.These electronic states are scattered by low-frequency phonons arising from mixed vibrations of Li and Al affected by ISQs to enhance electron–phonon coupling.Our study largely expands the research scope of electrides,provides new insight for understanding phase transitions,and elucidates the effects of ISQs on superconducting behavior.
基金supported in part by the National Key R&D Program of China (Contract Nos.2023YFA1606500,2024YFE0109800,and 2024YFE0110400)Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB34010000)+5 种基金the Gansu Key Project of Science and Technology (Grant No.23ZDGA014)the Guangdong Major Project of Basic and Applied Basic Research (Grant No.2021B0301030006)the National Natural Science Foundation of China (Grant Nos.12105328,W2412040,12475126,12422507,12035011,12375118,12435008,and W2412043)the Chinese Academy of Sciences Project for Young Scientists in Basic Research(Grant No.YSBR-002)the Youth Innovation Promotion Association of the Chinese Academy of Sciences (Grant Nos.2020409 and 2023439)the Russian Science Foundation (Grant No.25-42-00003)。
文摘We report the results of the experiment on synthesizing ^(287,288)Mc isotopes (Z=115) using the fusionevaporation reaction ^(243)Am(^(48)Ca,4n,3n)^(287,288)Mc at the Spectrometer for Heavy Atoms and Nuclear Structure-2(SHANS2),a gas-filled recoil separator located at the China Accelerator Facility for Superheavy Elements(CAFE2).In total,20 decay chains are attributed to ^(288)Mc and 1 decay chain is assigned to ^(287)Mc.The measured oa-decay properties of ^(287,288)Mc as well as its descendants are consistent with the known data.No additional decay chains originating from the 2n or 5n reaction channels were detected.The excitation function of the ^(243)Am(^(48)Ca,3n)^(288)Mc reaction was measured at the cross-section level of picobarn,which indicates the promising capability for the study of heavy and superheavy nuclei at the facility.
基金Project supported by the Science and Technology Project of State Grid Corporation of China(Grant No.5700-202355839A-4-3-WL).
文摘This paper presents the high-order nonlinear spectrum of six-wave mixing(SWM)influenced by ionizing Rydberg atom environment in rubidium thermal vapor.The experimentally measured transmitted SWM signals reveal significant spectrum shifts and novel regularities,providing nonlinear spectrum insights into the ionization characteristics of Rydberg atoms.The detailed spectrum variations with increasing ion density are presented,paving the way for multi-wave mixing distribution of plasma and demonstrating SWM’s potential as a tool for measuring the electric field induced by the ionization process.
基金supported by the National Natural Science Foundation of China(Nos.U22B2067 and 52073176).
文摘350 keV He^(+) ions were injected into laser powder bed fusion(LPBF)-processed 304L stainless steel and traditional rolled 304L stainless steel with a flux of 1×10^(17) ions/cm^(2) at room temperature,followed by annealing at 750℃ for 10,100,and 300 h,respectively.The results showed that material swelling due to helium bubble coarsening was almost not observed in either the LPBF or rolled samples after 10 h of annealing duration.Rapid coarsening and swelling of bubbles occurred in the rolled samples,but only moderate bubble growth occurred in the LPBF sample after annealing for 100 h.After annealing for 300 h,the helium bubbles in both samples tended to grow steadily.For 10 h of annealing,the irradiated samples were in a disequilibrium state,and the apparent activation energy(E^(act))calculated by the Arrhenius model determined that helium atoms tended to diffuse through the displacement mechanism,and helium bubbles grew under the migration and coalescence(MC)mechanism.With annealing times over 100 h,the high-density dislocations and nano-oxide particles in the LPBF sample still had a strong trapping effect on the movement and growth of helium bubbles.After annealing for 300 h,the cellular subgrains in the LPBF sample decomposed,and the nano-oxide particles had no trapping effect on the helium bubbles.At this time,the dislocation structure played a primary role in suppressing the growth of helium bubbles,and the radiation resistance of the LPBF sample remained superior to that of the rolled samples.
