The Dynamical Density Functional Theory(DDFT)algorithm,derived by associating classical Density Functional Theory(DFT)with the fundamental Smoluchowski dynamical equation,describes the evolution of inhomo-geneous flui...The Dynamical Density Functional Theory(DDFT)algorithm,derived by associating classical Density Functional Theory(DFT)with the fundamental Smoluchowski dynamical equation,describes the evolution of inhomo-geneous fluid density distributions over time.It plays a significant role in studying the evolution of density distributions over time in inhomogeneous systems.The Sunway Bluelight II supercomputer,as a new generation of China’s developed supercomputer,possesses powerful computational capabilities.Porting and optimizing industrial software on this platform holds significant importance.For the optimization of the DDFT algorithm,based on the Sunway Bluelight II supercomputer and the unique hardware architecture of the SW39000 processor,this work proposes three acceleration strategies to enhance computational efficiency and performance,including direct parallel optimization,local-memory constrained optimization for CPEs,and multi-core groups collaboration and communication optimization.This method combines the characteristics of the program’s algorithm with the unique hardware architecture of the Sunway Bluelight II supercomputer,optimizing the storage and transmission structures to achieve a closer integration of software and hardware.For the first time,this paper presents Sunway-Dynamical Density Functional Theory(SW-DDFT).Experimental results show that SW-DDFT achieves a speedup of 6.67 times within a single-core group compared to the original DDFT implementation,with six core groups(a total of 384 CPEs),the maximum speedup can reach 28.64 times,and parallel efficiency can reach 71%,demonstrating excellent acceleration performance.展开更多
Efficient surface passivation is critical for achieving high-performance perovskite solar cells(PSCs),yet the discovery of optimal passivators remains a time-consuming,trial-and-error process.Here,we report a synergis...Efficient surface passivation is critical for achieving high-performance perovskite solar cells(PSCs),yet the discovery of optimal passivators remains a time-consuming,trial-and-error process.Here,we report a synergistic machine learning(ML)and density functional theory(DFT)approach that enables predictive and rapid identification of effective passivation materials.By training an XGBoost model(91.3%accuracy)with DFT-derived molecular descriptors and activity calculations,we identify 2-(4-aminophenyl)-3H-benzimidazol-5-amine(APBIA)as a promising passivator.Experimental validation demonstrates that APBIA effectively removes surface impurities and passivates defects within perovskite films,leading to a significant increase in power conversion efficiency(PCE)from 22.48%to 25.55%(certified as 25.02%).This ML-DFT framework provides a generalizable pathway for accelerating the development of advanced functional materials for photovoltaic applications.展开更多
Density functional theory(DFT)calculations were employed to investigate the adsorption behavior of NH_(3),AsH_(3),PH_(3),CO_(2),and CH_(4)molecules on both pristine and mono-vacancy phosphorene sheets.The pristine pho...Density functional theory(DFT)calculations were employed to investigate the adsorption behavior of NH_(3),AsH_(3),PH_(3),CO_(2),and CH_(4)molecules on both pristine and mono-vacancy phosphorene sheets.The pristine phosphorene surface showsweak physisorption with all the gasmolecules,inducing onlyminor changes in its structural and electronic properties.However,the introduction ofmono-vacancies significantly enhances the interaction strength with NH_(3),PH_(3),CO_(2),and CH_(4).These variations are attributed to substantial charge redistribution and orbital hybridization in the presence of defects.The defective phosphorene sheet also exhibits enhanced adsorption energies,along with favorable sensitivity and recovery characteristics,highlighting its potential as a promising gas sensor for NH_(3),AsH_(3),PH_(3),CO_(2),and CH_(4)at ambient conditions.展开更多
Machine learning(ML)is recognized as a potent tool for the inverse design of environmental functional material,particularly for complex entities like biochar-based catalysts(BCs).Thus,the tailored BCs can have a disti...Machine learning(ML)is recognized as a potent tool for the inverse design of environmental functional material,particularly for complex entities like biochar-based catalysts(BCs).Thus,the tailored BCs can have a distinct ability to trigger the nonradical pathway in advance oxidation processes(AOPs),promising a stable,rapid and selective degradation of persistent contaminants.However,due to the inherent“black box”nature and limitations of input features,results and conclusions derived from ML may not always be intuitively understood or comprehensively validated.To tackle this challenge,we linked the front-point interpretable analysis approaches with back-point density functional theory(DFT)calculations to form a chained learning strategy for deeper sight into the intrinsic activation mechanism of BCs in AOPs.At the front point,we conducted an easy-to-interpret meta-analysis to validate two strategies for enhancing nonradical pathways by increasing oxygen content and specific surface area(SSA),and prepared oxidized biochar(OBC500)and SSA-increased biochar(SBC900)by controlling pyrolysis conditions and modification methods.Subsequently,experimental results showed that OBC500 and SBC900 had distinct dominant degradation pathways for 1O2 generation and electron transfer,respectively.Finally,at the end point,DFT calculations revealed their active sites and degradation mechanisms.This chained learning strategy elucidates fundamental principles for BC inverse design and showcases the exceptional capacity to integrate computational techniques to accelerate catalyst inverse design.展开更多
[Objectives]To investigate the effects of different planting densities and nitrogen application rates on the yield and quality of the tobacco cultivar Chuxue 80.[Methods]A field experiment was conducted in Hubei Provi...[Objectives]To investigate the effects of different planting densities and nitrogen application rates on the yield and quality of the tobacco cultivar Chuxue 80.[Methods]A field experiment was conducted in Hubei Province,evaluating various combinations of planting density and nitrogen rate for Chuxue 80.[Results]At the maturity stage,the TN1 treatment(5 kg N per 667 m^(2) with a density of 1900 plants per 667 m^(2))demonstrated the most favorable agronomic performance.The TN9 treatment(11 kg N per 667 m^(2) with a density of 1110 plants per 667 m^(2))achieved the highest wrapper tobacco yield and output value.Meanwhile,the TN5 treatment(8 kg N per 667 m^(2) with a density of 1515 plants per 667 m^(2))resulted in the best smoking quality.[Conclusions]The TN9 treatment,with a planting density of 1110 plants per 667 m^(2) and a nitrogen application rate of 11 kg per 667 m^(2),is recommended as the optimal cultivation practice for Chuxue 80 in Hubei Province.展开更多
Dielectric ceramic capacitors have attracted significant interest in advanced pulsed power systems owing to their ultrahigh power density and fast charge/discharge capabilities. The low breakdown strength(E_(b)) of di...Dielectric ceramic capacitors have attracted significant interest in advanced pulsed power systems owing to their ultrahigh power density and fast charge/discharge capabilities. The low breakdown strength(E_(b)) of dielectric ceramics poses a major bottleneck for achieving high recoverable energy storage density(W rec). In this study, using ingenious chemical component design, we achieved an ultrahigh Eb of 800 kV/cm and an excellent W rec value of 9.48 J/cm^(3) in the simple component 0.92NaNbO_(3)–0.08SmFeO_(3) ceramic. Finite element simulations corroborate that the optimized grain boundary network enables more uniform electric field distribution and effective suppression of breakdown propagation. The superior energy storage characteristics originate from two synergistic mechanisms:(Ι) the incorporation of SmFeO_(3) suppresses grain growth, resulting in refined microstructure with increased grain boundary density that substantially enhances E_(b);(II) the introduction of Sm^(3+) and Fe^(3+) ions causes a mismatch between the A/B site ions, inducing lattice distortion and high disorder, which enhances the local random fields and relaxor behavior. This study establishes a promising pathway for designing high-energy-density dielectric ceramic capacitors.展开更多
Although traditional gamma-gamma density(GGD)logging technology is widely utilized,its potential environmental risks have prompted the development of more environmentally friendly neutron-gamma density(NGD)logging tec...Although traditional gamma-gamma density(GGD)logging technology is widely utilized,its potential environmental risks have prompted the development of more environmentally friendly neutron-gamma density(NGD)logging technology.However,NGD measurements are influenced by both neutron and gamma radiations.In the logging environment,variations in the formation composition indicate different elemental compositions,which affect the neutron-gamma reaction cross-sections and gamma generation.Compared to traditional gamma sources such as Cs-137,these changes significantly affect the generation and transport of neutron-induced inelastic gamma rays and hinder accurate measurements.To address this,a novel method is proposed that incorporates the mass attenuation coefficient function to account for the effects of various lithologies and pore contents on gamma-ray attenuation,thereby achieving more accurate density measurements by clarifying the transport processes of inelastic gamma rays with varying energies and spatial distributions in varied logging environments.The proposed method avoids the complex correction of neutron transport and is verified through Monte Carlo simulations for its applicability across various lithologies and pore contents,demonstrating absolute density errors that are less than 0.02 g/cm^(3)in clean formations and indicating good accuracy.This study clarifies the NGD mechanism and provides theoretical guidance for the application of NGD logging methods.Further studies will be conducted on extreme environmental conditions and tool calibration.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
The purpose is to explore the effects of Exercise rehabilitation(ER)on bone mineral density(BMD)of the knee,muscle strength(MS),and physical function(PF)after ACL rupture.Finally,A total of 58 patients were randomized...The purpose is to explore the effects of Exercise rehabilitation(ER)on bone mineral density(BMD)of the knee,muscle strength(MS),and physical function(PF)after ACL rupture.Finally,A total of 58 patients were randomized into 2 groups(Control Group[CON]:conventional treatment,male=16,female=13,age=[31.63±8.01]years;Exercise rehabilitation group[ER]:6-week ER on CON basis,male=17,female=12,age=[31.26±7.07]years).At baseline and 6 weeks,the knee BMD was measured using DEXA,MS and PF measures were recorded by isokinetic strength test,IKDC,Lysholm,and VAS score.T-tests,analysis of variance(ANOVA),and Mann-Whitney tests were used for comparisons.The BMD outcomes:after a 6-week period,the BMD of the CON([1.47±0.24]g·cm^(-2))was significantly lower than that of the ER([1.65±0.37]g·cm^(-2))at lateral condyle of femur(LCF)(p=0.041).MS outcomes:at 6 weeks,the relative peak torque(RPT)of the quadriceps and hamstrings during concentric contractions in ER group were significantly higher than that in CON group(p<0.001,p=0.017).Similarly,during eccentric contractions in ER group,the RPT of the quadriceps and the H/Q ratio revealed significant variations from the CON group(p=0.033,p=0.043).PF outcomes:the IKDC,Lysholm,and VAS scores of the ER group were significantly improved compared to the CON group(p<0.001,p<0.001,p=0.002).The conclusion is that 6 weeks of ER intervention for patients with ACL rupture can effectively delay the decline of BMD in the LCF of the knee joint,and enhance the restoration of MS and PF.This provides guidance for clinical rehabilitation.展开更多
Cu_(x)Ta_(2-x)O_(5) compositions were investigated for advanced thermoelectric and optical applications,using both simulations and experimental approaches.Density functional theory calculations were performed before t...Cu_(x)Ta_(2-x)O_(5) compositions were investigated for advanced thermoelectric and optical applications,using both simulations and experimental approaches.Density functional theory calculations were performed before the experimental observations to predict the trends of various parameters.Crystal structure analysis confirmed the presence of the orthorhombic Ta_(2)O_(5) phase in all the compositions.The composition and morphology demonstrated impurity-free contents with uniform and crack-free surfaces.Thermoelectric analysis depicted a decrease in Seebeck coefficient from 3.66??V·K^(-1)to 1.91??V·K^(-1)and an increase in the value of specific heat from 0.73 J·K^(-1)·kg^(-1)to 11.6 J·K^(-1)·kg^(-1)upon Cu incorporation in structure.The bandgap was found to reduce from 2.61 to 1.38 e V with Cu-induced electronic states.The real epsilon and static refractive index increased from 3.75 to 4.57 and from 1.93 to 2.11,respectively,with increment in Cu content.The enhanced parameters,focusing on the thermoelectric and optical responses,make these compositions potential candidates for advanced optoelectronic applications.展开更多
Insight into the carbon turnover in soil aggregates and density fractions is essential for reducing the uncertainty in estimating carbon pools on the Tibetan Plateau,and how they vary with land use type is unclear.In ...Insight into the carbon turnover in soil aggregates and density fractions is essential for reducing the uncertainty in estimating carbon pools on the Tibetan Plateau,and how they vary with land use type is unclear.In this study,the effect of land use type on carbon storage and fractionation was quantified based on organic carbon and its ^(13)C abundance at the microscale of soil aggregates and density fractions in Tibetan alpine ecosystems.The sequence of soil aggregate destruction in the land use types of plantation(13.1%)<shrubland(32.7%)<grassland(47.9%)<farmland(61.8%)shows that plantations strengthen the soil structure.Plantation land had a greater contribution of light fraction organic carbon(28.3%)but a lower contribution of mineral-associated organic carbon(40.6%)to the carbon stock compared to farmland(13.5 and 70.3%).Interestingly,plantation land enhanced the aggregational differentiation of organic carbon and ^(13)C in each density fraction,whereas no such phenomenon existed in the soil organic carbon.Carbon isotope analyses revealed that carbon transfer in the plantation land occurred from the light fraction in macroaggregates(–24.9‰)to the mineral-associated fraction in microaggregates(–19.9‰).When compared to the other three land use types,the low transferability of carbon in aggregates and density fractions in plantation land provides a stable carbon pool for the Tibetan Plateau.This study shows that plantations can mitigate global climate change by slowing carbon transfer and increasing carbon storage at the microscale of aggregates and density fractions in alpine regions.展开更多
The rapid recombination of photogenerated charge carriers and the poor stability of metal sulfides remain bottlenecks limiting their practical applications. In this study, sulfur vacancies were introduced into an S-sc...The rapid recombination of photogenerated charge carriers and the poor stability of metal sulfides remain bottlenecks limiting their practical applications. In this study, sulfur vacancies were introduced into an S-scheme AgIn_(5)S_(8)/Bi_(2)S_(3) heterojunction via an in situ hydrothermal method. The sulfur vacancies induced charge density redistribution within the heterojunction and generated efficient active sites for electrons, thereby creating a localized electron-rich environment. The synergistic effects of the sulfur vacancies, internal electric field, and defect energy levels accelerated the separation and transfer of photogenerated charge carriers via the S-scheme pathway, thereby enhancing the visible-light photocatalytic performance, by achieving a Cr(Ⅵ) reduction efficiency of 99.6%. More importantly, the long-term stability and excellent anti-interference capability of the S-scheme AgIn_(5)S_(8)/Bi_(2)S_(3) heterojunction demonstrate its practical application potential, achieving 98.9% Cr(Ⅵ) removal from real electroplating wastewater and meeting discharge standards. This work provides a theoretical basis for constructing highly-catalytic S-scheme heterojunctions and serves as a promising solution for Cr(VI)-containing electroplating wastewater treatment.展开更多
The stress-strain behavior of calcareous sand is significantly influencedby particle breakage(B)and initial relative density(Dri),but few constitutive models consider their combined effects.To bridge this gap,we condu...The stress-strain behavior of calcareous sand is significantly influencedby particle breakage(B)and initial relative density(Dri),but few constitutive models consider their combined effects.To bridge this gap,we conducted a series of triaxial tests on calcareous sand with varying Dri and stress paths,examining particle breakage and critical state behavior.Key findingsinclude:(1)At a constant stress ratio(η),B follows a hyperbolic relationship with mean effective stress(p'),and for a given p',B increases proportionally withη;(2)The critical state line(CSL)moves downward with increasing Dri,whereas the critical state friction angle(φcs)decreases with increasing B.Based on these findings,we propose a unifiedbreakage evolution model to quantify particle breakage in calcareous sand under various loading conditions.Integrating this model with the Normal Consolidation Line(NCL)and CSL equations,we successfully simulate the steepening of NCL and CSL slopes as B increases with the onset of particle breakage.Furthermore,we quantitatively evaluate the effect of B onφcs.Finally,within the framework of Critical State Soil Mechanics and Hypoplasticity theory,we develop a hypoplastic model incorporating B and Dri.The model is validated through strong agreement with experimental results across various initial relative densities,stress paths and drainage conditions.展开更多
Exploring high-performance electrocatalysts for the nitrate reduction reaction(NO_(3)RR)is crucial for environmental nitrate removal and ammonia synthesis.Single-atom collaboration with cluster can provide sufficient ...Exploring high-performance electrocatalysts for the nitrate reduction reaction(NO_(3)RR)is crucial for environmental nitrate removal and ammonia synthesis.Single-atom collaboration with cluster can provide sufficient active sites for catalysts to promote NO_(3)RR,yet the unclear synergistic effect between the two hinders their rational design.Herein,a series of Ir_(3)clusters and metal single atoms co-embedded in graphitic carbon nitride(g-CN)catalysts(Ir_(3)M1)were constructed,and the synergistic effects of Ir_(3)clusters and M1 single atoms on the NO_(3)RR catalytic mechanism and activity were systematically explored using density functional theory(DFT)calculations combined with machine learning.Comprehensive evaluations of structural stability and catalytic activity demonstrate that the synergy between single atoms and clusters effectively balances the adsorption energies of key intermediates,yielding exceptional catalytic performance(the limiting potential of Ir_(3)Ti_(1)can reach−0.22 V).Machine learning models further clarify the synergistic mechanism,where the geometric configurations of clusters serve as critical features for modulating the catalytic activity of single-atom sites,whereas the electronic structures of single atoms directly govern the reactivity of cluster sites.This DFT-machine learning approach provides theoretical guidelines for catalyst design and a predictive framework for efficient NO_(3)RR electrocatalysts.展开更多
In this study,we analyze the impact of the May 2024 geomagnetic storm on the thermospheric mass density by using TianMu-1 constellation satellite(TM02,TM06,TM07,TM11,TM15)observations.These observations reveal intense...In this study,we analyze the impact of the May 2024 geomagnetic storm on the thermospheric mass density by using TianMu-1 constellation satellite(TM02,TM06,TM07,TM11,TM15)observations.These observations reveal intense large-scale traveling atmospheric disturbances(TADs)originating at high latitudes and propagating equatorward.Observations by TM02 captured the evolution of a TAD structure:An initial amplitude of~3.89×10^(-12)kg/m^(3)at hundred-kilometer scale subsequently intensified to 4.78×10^(-12)kg/m^(3),with the spatial extent expanding to the thousand-kilometer level.Significant hemispheric asymmetry was observed:the absolute density was higher predominantly in the northern hemisphere(TM02,TM06,TM07,TM11),whereas the difference in the relative density consistently showed greater enhancements in the southern hemisphere across all satellites,with the maximum north-south density differences exceeding 195%-640%above 60°latitude.In conjunction with SuperDARN(Super Dual Auroral Radar Network)observations,this striking hemispheric asymmetry can likely be attributed to disparities in plasma convection patterns between the two hemispheres.Furthermore,density perturbation characteristics exhibited strong local time(LT)dependence:Near noon(~10.7 LT,TM02 descending),the northern hemisphere onset preceded the southern onset.Conversely,near dusk(~17.6 LT,TM15 descending),the southern onset led the northern onset by approximately 3 hours.Ascending orbits(TM02,TM06,TM07,TM15)typically yielded larger global density enhancements compared with smaller southern-confined enhancements during descending orbits.Satellite TM11 showed comparable perturbations in both ascending and descending orbits.By leveraging its unique orbital architecture,the TianMu-1 constellation enables global near-simultaneous multi-LT sampling,providing a robust data foundation for both scientific research and engineering applications.展开更多
Soil respiration is the key process driving CO_(2) exchange between forest soils and the atmosphere and regulated by soil organic carbon(SOC)characteristics and extracellular enzyme activities.However,the direction an...Soil respiration is the key process driving CO_(2) exchange between forest soils and the atmosphere and regulated by soil organic carbon(SOC)characteristics and extracellular enzyme activities.However,the direction and magnitude of the effects of stand density on labile SOC fractions,extracellular enzymes,and soil respiration across plantation ages remain unclear.We constructed enhanced soil respiration models using heterogeneous soil data under density regulation to better characterize soil processes.Study plots encompassing stand-density gradients were implemented in Larix principis-rupprechtii plantations spanning three age-class strata.During the growing season,systematic measurements were conducted on soil respiration rates,labile organic carbon fractions,and extracellular enzyme activities.A process-driven soil respiration model was developed by integrating nonlinear mixed-effects modeling frameworks with measured data.The moderate density stands showed increases in soil respiration(Rs),microbial biomass carbon(MBC),light fraction organic carbon(LFOC),β-1,4-glucosidase(BGC),andβ-N-acetyl glycosaminidase+leucine aminopeptidase(NAG+LAP).In 36a and 48a stands,the moderate-density stands NAG+LAP had a~35%increase compared to other density levels,while readily oxidized carbon(ROC)concentrations showed a significant~30%-50%reduction.All labile organic carbon components were stable with age,so that soil microorganisms were promoted to acquire C,N,and P.Temperature,moisture,MBC,BGC,and NAG+LAP were essential factors that affected soil respiration.Stand density has important impacts on soil respiration as it regulates the soil organic carbon and activities of extracellular enzymes.The roles of temperature,microbial biomass carbon,soil organic carbon and dissolved organic carbon are complex and directly affect autotrophic and heterotrophic respiration and regulate soil respiration by influencing microbial C and N acquisition.A mixed-effects model with nested stand density and age mathematically optimized the soil respiration model,enabling enhanced characterization of covariation patterns of soil respiration with related soil carbon pool variables.展开更多
基金supported by National Key Research and Development Program of China under Grant 2024YFE0210800National Natural Science Foundation of China under Grant 62495062Beijing Natural Science Foundation under Grant L242017.
文摘The Dynamical Density Functional Theory(DDFT)algorithm,derived by associating classical Density Functional Theory(DFT)with the fundamental Smoluchowski dynamical equation,describes the evolution of inhomo-geneous fluid density distributions over time.It plays a significant role in studying the evolution of density distributions over time in inhomogeneous systems.The Sunway Bluelight II supercomputer,as a new generation of China’s developed supercomputer,possesses powerful computational capabilities.Porting and optimizing industrial software on this platform holds significant importance.For the optimization of the DDFT algorithm,based on the Sunway Bluelight II supercomputer and the unique hardware architecture of the SW39000 processor,this work proposes three acceleration strategies to enhance computational efficiency and performance,including direct parallel optimization,local-memory constrained optimization for CPEs,and multi-core groups collaboration and communication optimization.This method combines the characteristics of the program’s algorithm with the unique hardware architecture of the Sunway Bluelight II supercomputer,optimizing the storage and transmission structures to achieve a closer integration of software and hardware.For the first time,this paper presents Sunway-Dynamical Density Functional Theory(SW-DDFT).Experimental results show that SW-DDFT achieves a speedup of 6.67 times within a single-core group compared to the original DDFT implementation,with six core groups(a total of 384 CPEs),the maximum speedup can reach 28.64 times,and parallel efficiency can reach 71%,demonstrating excellent acceleration performance.
基金supported by the National Key Research and Development Program of China (Grant No. 2024YFB4205101)the National Natural Science Foundation of China (No. 62274098 and No. 62074084)+2 种基金the Natural Science Foundation of Tianjin (No.22JCYBJC01300, No. 23JCYBJC01620 and No. 21JCYBJC00270)the Overseas Expertise Introduction Project for Discipline Innovation of Higher Edu cation of China (Grant No. B16027)the Fundamental Research Funds for the Central Universities,Nankai University (No. 63241568)
文摘Efficient surface passivation is critical for achieving high-performance perovskite solar cells(PSCs),yet the discovery of optimal passivators remains a time-consuming,trial-and-error process.Here,we report a synergistic machine learning(ML)and density functional theory(DFT)approach that enables predictive and rapid identification of effective passivation materials.By training an XGBoost model(91.3%accuracy)with DFT-derived molecular descriptors and activity calculations,we identify 2-(4-aminophenyl)-3H-benzimidazol-5-amine(APBIA)as a promising passivator.Experimental validation demonstrates that APBIA effectively removes surface impurities and passivates defects within perovskite films,leading to a significant increase in power conversion efficiency(PCE)from 22.48%to 25.55%(certified as 25.02%).This ML-DFT framework provides a generalizable pathway for accelerating the development of advanced functional materials for photovoltaic applications.
基金financial support to conduct this research from the Science and Engineering Research Board(SERB)through a state university research excellence(SURE)grant(SUR/2022/004935).
文摘Density functional theory(DFT)calculations were employed to investigate the adsorption behavior of NH_(3),AsH_(3),PH_(3),CO_(2),and CH_(4)molecules on both pristine and mono-vacancy phosphorene sheets.The pristine phosphorene surface showsweak physisorption with all the gasmolecules,inducing onlyminor changes in its structural and electronic properties.However,the introduction ofmono-vacancies significantly enhances the interaction strength with NH_(3),PH_(3),CO_(2),and CH_(4).These variations are attributed to substantial charge redistribution and orbital hybridization in the presence of defects.The defective phosphorene sheet also exhibits enhanced adsorption energies,along with favorable sensitivity and recovery characteristics,highlighting its potential as a promising gas sensor for NH_(3),AsH_(3),PH_(3),CO_(2),and CH_(4)at ambient conditions.
基金supported by Project of National and Local Joint Engineering Research Center for Biomass Energy Development and Utilization(Harbin Institute of Technology,No.2021A004).
文摘Machine learning(ML)is recognized as a potent tool for the inverse design of environmental functional material,particularly for complex entities like biochar-based catalysts(BCs).Thus,the tailored BCs can have a distinct ability to trigger the nonradical pathway in advance oxidation processes(AOPs),promising a stable,rapid and selective degradation of persistent contaminants.However,due to the inherent“black box”nature and limitations of input features,results and conclusions derived from ML may not always be intuitively understood or comprehensively validated.To tackle this challenge,we linked the front-point interpretable analysis approaches with back-point density functional theory(DFT)calculations to form a chained learning strategy for deeper sight into the intrinsic activation mechanism of BCs in AOPs.At the front point,we conducted an easy-to-interpret meta-analysis to validate two strategies for enhancing nonradical pathways by increasing oxygen content and specific surface area(SSA),and prepared oxidized biochar(OBC500)and SSA-increased biochar(SBC900)by controlling pyrolysis conditions and modification methods.Subsequently,experimental results showed that OBC500 and SBC900 had distinct dominant degradation pathways for 1O2 generation and electron transfer,respectively.Finally,at the end point,DFT calculations revealed their active sites and degradation mechanisms.This chained learning strategy elucidates fundamental principles for BC inverse design and showcases the exceptional capacity to integrate computational techniques to accelerate catalyst inverse design.
基金Supported by Science and Technology Project of China Tobacco Zhejiang Industrial Co.,Ltd.(2023330000340093).
文摘[Objectives]To investigate the effects of different planting densities and nitrogen application rates on the yield and quality of the tobacco cultivar Chuxue 80.[Methods]A field experiment was conducted in Hubei Province,evaluating various combinations of planting density and nitrogen rate for Chuxue 80.[Results]At the maturity stage,the TN1 treatment(5 kg N per 667 m^(2) with a density of 1900 plants per 667 m^(2))demonstrated the most favorable agronomic performance.The TN9 treatment(11 kg N per 667 m^(2) with a density of 1110 plants per 667 m^(2))achieved the highest wrapper tobacco yield and output value.Meanwhile,the TN5 treatment(8 kg N per 667 m^(2) with a density of 1515 plants per 667 m^(2))resulted in the best smoking quality.[Conclusions]The TN9 treatment,with a planting density of 1110 plants per 667 m^(2) and a nitrogen application rate of 11 kg per 667 m^(2),is recommended as the optimal cultivation practice for Chuxue 80 in Hubei Province.
基金supported by the National Natural Science Foundation of China (Grant Nos.52462018,52162019)the Key Project of the Natural Science Foundation of Jiangxi Province (Grant No.20252BAC250038)the Science Fund for Distinguished Young Scholars of Jiangxi Province (Grant No.20224ACB214007)。
文摘Dielectric ceramic capacitors have attracted significant interest in advanced pulsed power systems owing to their ultrahigh power density and fast charge/discharge capabilities. The low breakdown strength(E_(b)) of dielectric ceramics poses a major bottleneck for achieving high recoverable energy storage density(W rec). In this study, using ingenious chemical component design, we achieved an ultrahigh Eb of 800 kV/cm and an excellent W rec value of 9.48 J/cm^(3) in the simple component 0.92NaNbO_(3)–0.08SmFeO_(3) ceramic. Finite element simulations corroborate that the optimized grain boundary network enables more uniform electric field distribution and effective suppression of breakdown propagation. The superior energy storage characteristics originate from two synergistic mechanisms:(Ι) the incorporation of SmFeO_(3) suppresses grain growth, resulting in refined microstructure with increased grain boundary density that substantially enhances E_(b);(II) the introduction of Sm^(3+) and Fe^(3+) ions causes a mismatch between the A/B site ions, inducing lattice distortion and high disorder, which enhances the local random fields and relaxor behavior. This study establishes a promising pathway for designing high-energy-density dielectric ceramic capacitors.
基金supported by the National Natural Science Foundation of China(U23B20151 and 52171253).
文摘Although traditional gamma-gamma density(GGD)logging technology is widely utilized,its potential environmental risks have prompted the development of more environmentally friendly neutron-gamma density(NGD)logging technology.However,NGD measurements are influenced by both neutron and gamma radiations.In the logging environment,variations in the formation composition indicate different elemental compositions,which affect the neutron-gamma reaction cross-sections and gamma generation.Compared to traditional gamma sources such as Cs-137,these changes significantly affect the generation and transport of neutron-induced inelastic gamma rays and hinder accurate measurements.To address this,a novel method is proposed that incorporates the mass attenuation coefficient function to account for the effects of various lithologies and pore contents on gamma-ray attenuation,thereby achieving more accurate density measurements by clarifying the transport processes of inelastic gamma rays with varying energies and spatial distributions in varied logging environments.The proposed method avoids the complex correction of neutron transport and is verified through Monte Carlo simulations for its applicability across various lithologies and pore contents,demonstrating absolute density errors that are less than 0.02 g/cm^(3)in clean formations and indicating good accuracy.This study clarifies the NGD mechanism and provides theoretical guidance for the application of NGD logging methods.Further studies will be conducted on extreme environmental conditions and tool calibration.
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provided by the Joint Fund for Regional Innovation and Development(U23A20471)Beijing Natural Science Foundation(L242161,L241073,and 7232354)。
文摘The purpose is to explore the effects of Exercise rehabilitation(ER)on bone mineral density(BMD)of the knee,muscle strength(MS),and physical function(PF)after ACL rupture.Finally,A total of 58 patients were randomized into 2 groups(Control Group[CON]:conventional treatment,male=16,female=13,age=[31.63±8.01]years;Exercise rehabilitation group[ER]:6-week ER on CON basis,male=17,female=12,age=[31.26±7.07]years).At baseline and 6 weeks,the knee BMD was measured using DEXA,MS and PF measures were recorded by isokinetic strength test,IKDC,Lysholm,and VAS score.T-tests,analysis of variance(ANOVA),and Mann-Whitney tests were used for comparisons.The BMD outcomes:after a 6-week period,the BMD of the CON([1.47±0.24]g·cm^(-2))was significantly lower than that of the ER([1.65±0.37]g·cm^(-2))at lateral condyle of femur(LCF)(p=0.041).MS outcomes:at 6 weeks,the relative peak torque(RPT)of the quadriceps and hamstrings during concentric contractions in ER group were significantly higher than that in CON group(p<0.001,p=0.017).Similarly,during eccentric contractions in ER group,the RPT of the quadriceps and the H/Q ratio revealed significant variations from the CON group(p=0.033,p=0.043).PF outcomes:the IKDC,Lysholm,and VAS scores of the ER group were significantly improved compared to the CON group(p<0.001,p<0.001,p=0.002).The conclusion is that 6 weeks of ER intervention for patients with ACL rupture can effectively delay the decline of BMD in the LCF of the knee joint,and enhance the restoration of MS and PF.This provides guidance for clinical rehabilitation.
基金the Deanship of Research and Graduate Studies at King Khalid University,Saudi Arabia,for funding this study through the Large Groups Project(Grant No.RGP2/2/47)the Deanship of Scientific Research at Northern Border University,Arar,KSA for funding this research work through project number NBU-FFR-2025-1902-02。
文摘Cu_(x)Ta_(2-x)O_(5) compositions were investigated for advanced thermoelectric and optical applications,using both simulations and experimental approaches.Density functional theory calculations were performed before the experimental observations to predict the trends of various parameters.Crystal structure analysis confirmed the presence of the orthorhombic Ta_(2)O_(5) phase in all the compositions.The composition and morphology demonstrated impurity-free contents with uniform and crack-free surfaces.Thermoelectric analysis depicted a decrease in Seebeck coefficient from 3.66??V·K^(-1)to 1.91??V·K^(-1)and an increase in the value of specific heat from 0.73 J·K^(-1)·kg^(-1)to 11.6 J·K^(-1)·kg^(-1)upon Cu incorporation in structure.The bandgap was found to reduce from 2.61 to 1.38 e V with Cu-induced electronic states.The real epsilon and static refractive index increased from 3.75 to 4.57 and from 1.93 to 2.11,respectively,with increment in Cu content.The enhanced parameters,focusing on the thermoelectric and optical responses,make these compositions potential candidates for advanced optoelectronic applications.
基金financially supported by the National Natural Science Foundation of China (42477044,32171648 and U23A2017)the Hubei Provincial Science and Technology Program,China (2025AFD451 and 2022CFB030)。
文摘Insight into the carbon turnover in soil aggregates and density fractions is essential for reducing the uncertainty in estimating carbon pools on the Tibetan Plateau,and how they vary with land use type is unclear.In this study,the effect of land use type on carbon storage and fractionation was quantified based on organic carbon and its ^(13)C abundance at the microscale of soil aggregates and density fractions in Tibetan alpine ecosystems.The sequence of soil aggregate destruction in the land use types of plantation(13.1%)<shrubland(32.7%)<grassland(47.9%)<farmland(61.8%)shows that plantations strengthen the soil structure.Plantation land had a greater contribution of light fraction organic carbon(28.3%)but a lower contribution of mineral-associated organic carbon(40.6%)to the carbon stock compared to farmland(13.5 and 70.3%).Interestingly,plantation land enhanced the aggregational differentiation of organic carbon and ^(13)C in each density fraction,whereas no such phenomenon existed in the soil organic carbon.Carbon isotope analyses revealed that carbon transfer in the plantation land occurred from the light fraction in macroaggregates(–24.9‰)to the mineral-associated fraction in microaggregates(–19.9‰).When compared to the other three land use types,the low transferability of carbon in aggregates and density fractions in plantation land provides a stable carbon pool for the Tibetan Plateau.This study shows that plantations can mitigate global climate change by slowing carbon transfer and increasing carbon storage at the microscale of aggregates and density fractions in alpine regions.
基金supported by the National Natural Science Foundation of China (Grant No.52470078)the Natural Science Foundation of Jiangxi Province (Grant No.20252BAC250042)the Key Laboratory of Jiangxi Province for Persistent Pollutants Prevention Control and Resource Reuse (Grant No.2023SSY02061)。
文摘The rapid recombination of photogenerated charge carriers and the poor stability of metal sulfides remain bottlenecks limiting their practical applications. In this study, sulfur vacancies were introduced into an S-scheme AgIn_(5)S_(8)/Bi_(2)S_(3) heterojunction via an in situ hydrothermal method. The sulfur vacancies induced charge density redistribution within the heterojunction and generated efficient active sites for electrons, thereby creating a localized electron-rich environment. The synergistic effects of the sulfur vacancies, internal electric field, and defect energy levels accelerated the separation and transfer of photogenerated charge carriers via the S-scheme pathway, thereby enhancing the visible-light photocatalytic performance, by achieving a Cr(Ⅵ) reduction efficiency of 99.6%. More importantly, the long-term stability and excellent anti-interference capability of the S-scheme AgIn_(5)S_(8)/Bi_(2)S_(3) heterojunction demonstrate its practical application potential, achieving 98.9% Cr(Ⅵ) removal from real electroplating wastewater and meeting discharge standards. This work provides a theoretical basis for constructing highly-catalytic S-scheme heterojunctions and serves as a promising solution for Cr(VI)-containing electroplating wastewater treatment.
基金support to this study from the National Natural Science Foundation of China,NSFC(Grant No.52278367)The Belt and Road Special Foundation of the National Key Laboratory ofWater Disaster Prevention(Grant No.2024nkms08).
文摘The stress-strain behavior of calcareous sand is significantly influencedby particle breakage(B)and initial relative density(Dri),but few constitutive models consider their combined effects.To bridge this gap,we conducted a series of triaxial tests on calcareous sand with varying Dri and stress paths,examining particle breakage and critical state behavior.Key findingsinclude:(1)At a constant stress ratio(η),B follows a hyperbolic relationship with mean effective stress(p'),and for a given p',B increases proportionally withη;(2)The critical state line(CSL)moves downward with increasing Dri,whereas the critical state friction angle(φcs)decreases with increasing B.Based on these findings,we propose a unifiedbreakage evolution model to quantify particle breakage in calcareous sand under various loading conditions.Integrating this model with the Normal Consolidation Line(NCL)and CSL equations,we successfully simulate the steepening of NCL and CSL slopes as B increases with the onset of particle breakage.Furthermore,we quantitatively evaluate the effect of B onφcs.Finally,within the framework of Critical State Soil Mechanics and Hypoplasticity theory,we develop a hypoplastic model incorporating B and Dri.The model is validated through strong agreement with experimental results across various initial relative densities,stress paths and drainage conditions.
基金the financial support from the Shandong Province colleges and universities youth innovation technology plan innovation team project(2022KJ285)the Natural Science Foundation of Shandong Province(ZR2022QE076)+1 种基金the National Natural Science Foundation of China(52202092)the Science and Technology Support Plan for Youth Innovation of Colleges and Universities of Shandong Province of China(2023KJ104).
文摘Exploring high-performance electrocatalysts for the nitrate reduction reaction(NO_(3)RR)is crucial for environmental nitrate removal and ammonia synthesis.Single-atom collaboration with cluster can provide sufficient active sites for catalysts to promote NO_(3)RR,yet the unclear synergistic effect between the two hinders their rational design.Herein,a series of Ir_(3)clusters and metal single atoms co-embedded in graphitic carbon nitride(g-CN)catalysts(Ir_(3)M1)were constructed,and the synergistic effects of Ir_(3)clusters and M1 single atoms on the NO_(3)RR catalytic mechanism and activity were systematically explored using density functional theory(DFT)calculations combined with machine learning.Comprehensive evaluations of structural stability and catalytic activity demonstrate that the synergy between single atoms and clusters effectively balances the adsorption energies of key intermediates,yielding exceptional catalytic performance(the limiting potential of Ir_(3)Ti_(1)can reach−0.22 V).Machine learning models further clarify the synergistic mechanism,where the geometric configurations of clusters serve as critical features for modulating the catalytic activity of single-atom sites,whereas the electronic structures of single atoms directly govern the reactivity of cluster sites.This DFT-machine learning approach provides theoretical guidelines for catalyst design and a predictive framework for efficient NO_(3)RR electrocatalysts.
基金the National Space Science Center (NSSC) of the Chinese Academy of Sciences for full support of this research workfunded by the Tian Mu-1 Constellation Atmospheric Density Detector (Grant No. E3C1162110)
文摘In this study,we analyze the impact of the May 2024 geomagnetic storm on the thermospheric mass density by using TianMu-1 constellation satellite(TM02,TM06,TM07,TM11,TM15)observations.These observations reveal intense large-scale traveling atmospheric disturbances(TADs)originating at high latitudes and propagating equatorward.Observations by TM02 captured the evolution of a TAD structure:An initial amplitude of~3.89×10^(-12)kg/m^(3)at hundred-kilometer scale subsequently intensified to 4.78×10^(-12)kg/m^(3),with the spatial extent expanding to the thousand-kilometer level.Significant hemispheric asymmetry was observed:the absolute density was higher predominantly in the northern hemisphere(TM02,TM06,TM07,TM11),whereas the difference in the relative density consistently showed greater enhancements in the southern hemisphere across all satellites,with the maximum north-south density differences exceeding 195%-640%above 60°latitude.In conjunction with SuperDARN(Super Dual Auroral Radar Network)observations,this striking hemispheric asymmetry can likely be attributed to disparities in plasma convection patterns between the two hemispheres.Furthermore,density perturbation characteristics exhibited strong local time(LT)dependence:Near noon(~10.7 LT,TM02 descending),the northern hemisphere onset preceded the southern onset.Conversely,near dusk(~17.6 LT,TM15 descending),the southern onset led the northern onset by approximately 3 hours.Ascending orbits(TM02,TM06,TM07,TM15)typically yielded larger global density enhancements compared with smaller southern-confined enhancements during descending orbits.Satellite TM11 showed comparable perturbations in both ascending and descending orbits.By leveraging its unique orbital architecture,the TianMu-1 constellation enables global near-simultaneous multi-LT sampling,providing a robust data foundation for both scientific research and engineering applications.
基金supported by the National Key Research and Development Program of China(2023YFD2200403)National Natural Science Foundation of China(No.32260382)the Natural Science Foundation of Guangxi(2025GXNSFBA069250).
文摘Soil respiration is the key process driving CO_(2) exchange between forest soils and the atmosphere and regulated by soil organic carbon(SOC)characteristics and extracellular enzyme activities.However,the direction and magnitude of the effects of stand density on labile SOC fractions,extracellular enzymes,and soil respiration across plantation ages remain unclear.We constructed enhanced soil respiration models using heterogeneous soil data under density regulation to better characterize soil processes.Study plots encompassing stand-density gradients were implemented in Larix principis-rupprechtii plantations spanning three age-class strata.During the growing season,systematic measurements were conducted on soil respiration rates,labile organic carbon fractions,and extracellular enzyme activities.A process-driven soil respiration model was developed by integrating nonlinear mixed-effects modeling frameworks with measured data.The moderate density stands showed increases in soil respiration(Rs),microbial biomass carbon(MBC),light fraction organic carbon(LFOC),β-1,4-glucosidase(BGC),andβ-N-acetyl glycosaminidase+leucine aminopeptidase(NAG+LAP).In 36a and 48a stands,the moderate-density stands NAG+LAP had a~35%increase compared to other density levels,while readily oxidized carbon(ROC)concentrations showed a significant~30%-50%reduction.All labile organic carbon components were stable with age,so that soil microorganisms were promoted to acquire C,N,and P.Temperature,moisture,MBC,BGC,and NAG+LAP were essential factors that affected soil respiration.Stand density has important impacts on soil respiration as it regulates the soil organic carbon and activities of extracellular enzymes.The roles of temperature,microbial biomass carbon,soil organic carbon and dissolved organic carbon are complex and directly affect autotrophic and heterotrophic respiration and regulate soil respiration by influencing microbial C and N acquisition.A mixed-effects model with nested stand density and age mathematically optimized the soil respiration model,enabling enhanced characterization of covariation patterns of soil respiration with related soil carbon pool variables.
