We performed a quantitative analysis of time-resolved laser-induced breakdown air plasma spectra to obtain the evolution of temperatures and species relative fractions.The air plasma was generated by focusing a 100 mJ...We performed a quantitative analysis of time-resolved laser-induced breakdown air plasma spectra to obtain the evolution of temperatures and species relative fractions.The air plasma was generated by focusing a 100 mJ Nd:YAG laser pulse,and the time-resolved spectra were recorded by an intensified charge-coupled device camera with incremental delay.The attention was mainly focused on the emission spectra of the first negative system of nitrogen(N_(2)^(+),B^(2)Σ-(u)^(-)-X^(2)Σ^(+)g)and the violet system of carbon nitride(CN,B^(2)Σ^(+)-X^(2)Σ^(+))located at 383-396 nm.A custom-built model was developed to perform the simulation and fitting of the N_(2)^(+)and the CN spectra from the air plasma.The model was verified by comparing to a published model with a 0.9860 Spearman correlation coefficient.With this model,the time-resolved non-equilibrium temperatures and relative fractions of N_(2)^(+)and CN were obtained with a fitting correlation coefficient higher than 0.9108.展开更多
Photoswitchable fluorescent polymeric nanoparticles were widely concerned because of their excellent features including the flexible design,easy preparation and functionalization,and thus exhibited great application p...Photoswitchable fluorescent polymeric nanoparticles were widely concerned because of their excellent features including the flexible design,easy preparation and functionalization,and thus exhibited great application potential in information encryption,anti-counterfeiting,but remained challenging in improving the security.Herein,we described a self-erased time-resolved information encryption via using photoswitchable dual-color fluorescent polymeric nanoparticles(PDFPNs)containing two fluorescence dyes(blue and red)and photochromic spiroxazine derivatives.In view of the different thermo-induced isomerization rates of photochromic spiroxazine derivatives in different flexible substrates,the decoloration rate of PDFPNs can be programmatically tuned by regulating ratio between rigid polymer and flexible polymer.Therefore,after ultraviolet light(UV)irradiation,correct information could only be recognized in preestablished time during the self-erased process.Our results indicated that PDFPNs exhibited fast photo-responsibility(2 min),high fluorescence contrast,well-pleasing photo-reversibility(>20 times),and programmable thermo-responsiveness(24 s-6 h).We thus demonstrated their application in the selferased time-resolved information encryption and anti-counterfeiting with high security.展开更多
Quantum materials have attracted a great deal of attention because of their rich landscape of electronic structures,topological phases,strong correlation effects,and exotic orders.These systems provide a fertile platf...Quantum materials have attracted a great deal of attention because of their rich landscape of electronic structures,topological phases,strong correlation effects,and exotic orders.These systems provide a fertile platform for the exploration of novel quantum phenomena and materials applications.Particularly exciting is the exploration of nonequilibrium dynamics in quantum materials,which has significant research and potential application values.Pump-probe techniques play a key role in revealing the dynamics of quantum materials on remarkably short timescales,providing an attractive yet challenging avenue of research.In this context,time-resolved x-ray as an emerging probe exhibits high time resolution,momentum resolution,and substantial momentum coverage.It can reveal unprecedented transient states,distinguish between entangled ordered states,and has a compelling potential to probe ultrafast dynamics in a wide variety of quantum materials.Despite its unique advantages,time-resolved x-ray scattering still faces several technological and methodological challenges.In this review,we highlight recent advances focusing on the use of time-resolved x-ray scattering to probe dynamic processes in quantum materials.We discuss representative examples across structural,electronic,magnetic,and lattice degrees of freedom,and outline promising directions for future research in this rapidly evolving field.展开更多
Time-resolved flow cytometry(TRFC)was used to measure metabolic differences in estrogen receptor-positive breast cancer cells.This specialty cytometry technique measures fluorescence lifetimes as a single-cell paramet...Time-resolved flow cytometry(TRFC)was used to measure metabolic differences in estrogen receptor-positive breast cancer cells.This specialty cytometry technique measures fluorescence lifetimes as a single-cell parameter thereby providing a unique approach for high-throughput cell counting and screening.Differences in fluorescence lifetime were detected and this was associated with sensitivity to the commonly prescribed therapeutic tamoxifen.Differences in fluorescence lifetime are attributed to the binding states of the autofluorescent metabolite NAD(P)H.The function of NAD(P)H is well described and in general involves cycling from a reduced to oxidized state to facilitate electron transport for the conversion of pyruvate to lactate.NAD(P)H fluorescence lifetimes depend on the bound or unbound state of the metabolite,which also relates to metabolic transitions between oxidative phosphorylation and glycolysis.To determine if fundamental metabolic profiles differ for cells that are sensitive to tamoxifen compared to those that are resistant,large populations of MCF-7 breast cancer cells were screened and fluorescence lifetimes were quantified.Additionally,metabolic differences associated with tamoxifen sensitivity were measured with a Seahorse HS mini metabolic analyzer(Agilent Technologies Inc.Santa Clara,CA)and confocal imaging.Results show that tamoxifen-resistant breast cancer cells have increased utilization of glycolysis for energy production compared to tamoxifen-sensitive breast cancer cells.This work is impacting because it establishes an early step toward developing a reliable screening technology in which large cell censuses can be differentiated for drug sensitivity in a label-free fashion.展开更多
In this paper,we consider the maximal positive definite solution of the nonlinear matrix equation.By using the idea of Algorithm 2.1 in ZHANG(2013),a new inversion-free method with a stepsize parameter is proposed to ...In this paper,we consider the maximal positive definite solution of the nonlinear matrix equation.By using the idea of Algorithm 2.1 in ZHANG(2013),a new inversion-free method with a stepsize parameter is proposed to obtain the maximal positive definite solution of nonlinear matrix equation X+A^(*)X|^(-α)A=Q with the case 0<α≤1.Based on this method,a new iterative algorithm is developed,and its convergence proof is given.Finally,two numerical examples are provided to show the effectiveness of the proposed method.展开更多
Objectives This review aimed to systematically synthesize the available research on the disclosure of diagnosis and related issues in childhood cancer from the perspectives of healthcare professionals,with the goal of...Objectives This review aimed to systematically synthesize the available research on the disclosure of diagnosis and related issues in childhood cancer from the perspectives of healthcare professionals,with the goal of informing the optimization of disclosure processes and meeting the communication needs of affected families.Methods In accordance with the Joanna Briggs Institute(JBI)methodology for mixed methods systematic reviews,the convergent segregated approach was used in this review.Articles were retrieved from 11 databases,including PubMed,Web of Science,CINAHL,CENTRAL,Embase,Ovid/Medline,PsycINFO,PsycArticles,Scopus,ERIC,and China National Knowledge Infrastructure(CNKI).The quality of the selected articles was assessed using the Mixed Method Appraisal Tool(MMAT).The review protocol was registered on PROSPERO(CRD42024542746).Results A total of 21 studies from 10 countries were included.Their methodological quality was generally medium to high,with MMAT scores ranging from 60%to 100%.The synthesis yielded three core themes:1)the spectrum of professional and societal attitudes toward disclosure;2)the dynamic practices of navigating disclosure amid uncertainty,including timing and environment,stakeholders,and content of disclosure;and 3)factors influencing disclosure,including children’s,parental,healthcare professionals’,and socio-cultural factors.Conclusions This review synthesized the perspectives and experiences of healthcare professionals regarding disclosure in childhood cancer,highlighting the complexity and multidimensional nature of this process in clinical practice.Future research should further investigate the experiences and needs of children and their parents,explore cultural variations in disclosure practices,develop context-appropriate assessment tools,and construct multidimensional intervention strategies to enhance the humanistic care and professional effectiveness of the disclosure process.展开更多
As binary geological media,soil-rock mixtures(SRMs)exhibit a distinct gradational composition,leading to their unique mechanical behaviors.To appraise the stability of SRM slopes,it is essential to determine equivalen...As binary geological media,soil-rock mixtures(SRMs)exhibit a distinct gradational composition,leading to their unique mechanical behaviors.To appraise the stability of SRM slopes,it is essential to determine equivalent parameters of SRMs,which are typically obtained through experimental and numerical methods.In contrasted to other numerical methods,the numerical manifold method(NMM)is more effective in addressing SRM problems.This is because the high-precision regular mathematical meshes in NMM can be used without aligning with the soil-rock interfaces and boundaries of SRMs.In the current research,the equivalent strength parameters of SRMs,i.e.the equivalent cohesion ce and internal friction angleϕ_(e),are determined using NMM.Initially,an NMM triaxial numerical model is established and validated based on triaxial experiments.Subsequently,the soil and rock parameters are derived through parameter inversion.Moreover,the impacts of rock content,size,shape and rock blocks'major-axis orientation on ce andϕ_(e) of SRMs are thoroughly examined using the NMM triaxial numerical model.Additionally,a fitting function is proposed to linkϕ_(e) to the rock content and size of SRMs.When other influencing factors are fixed,the above fitting model leads to the following conclusions:(1)the predictedϕ_(e) of SRMs increase with the increase of rock content;and(2)SRM samples with smaller rocks display a higher predictedϕ_(e).展开更多
The Good Wife is an American TV series that focuses on women’s independence,politics,and law.The drama has been remade in China,Japan,and South Korea.This research aims to use Nida’s Functional Equivalence Theory to...The Good Wife is an American TV series that focuses on women’s independence,politics,and law.The drama has been remade in China,Japan,and South Korea.This research aims to use Nida’s Functional Equivalence Theory to analyze the methods of its English-to-Chinese subtitle translation by considering social,cultural,and historic backgrounds between China and America.After data collection and case analysis,the study found that:(1)Five major translation methods are adopted in the subtitle translation of The Good Wife.They are free translation,variation,literal translation,addition,and omission.Among them,free translation is the most frequently used,while omission is used least.(2)The subtitle translation of films and TV series is limited by time and space restrictions,social-cultural differences,and other factors.When translating,translators should try to use humorous words,euphemism,intonation,and other ways,and combine different methods such as literal translation,free translation,variation,addition,omission,and other methods to seek equivalence both in the meaning and function of subtitles under the guidance of Functional Equivalence Theory.展开更多
Edible oil is one major nutritional ingredient to human and widely consumed directly. The contamination of aflatoxin B1 （AFB1） in edible oils has been attracted exten-sive efforts due to its hazard to human health a...Edible oil is one major nutritional ingredient to human and widely consumed directly. The contamination of aflatoxin B1 （AFB1） in edible oils has been attracted exten-sive efforts due to its hazard to human health and life. To avoid the digestion of edible oils contaminated by AFB1 the development of rapid and sensitive sensing method for AFB1 is required. Herein, a quantitative, sensitive and rapid method for AFB1 detection in edible oils was proposed by using ultrasensitive time-resolved fluorescent immunosensing （TRFIS） method. This method poses unique advantages from both time-resolved fluorescent sens-ing method and immunochromatographic assay format. The nanospheres were modified with fluorescent europium and then captured the home-made monoclonal antibody against AFB1 （3G1）. After optimization, by using a competitive immunosensing manner, this TRFIS method has a detectable linear range of 0.54-20.0 μg/kg with minimum detectable concen-tration of 0.18μg/kg. It can be completed merely within 10 min with recovery from 87.0% to 121.9%. The agreement was observed between the results by TRFIS and high perfor-mance liquid chromatography （HPLC） methods. This research provides a promising sens-ing method for sensitive and rapid determining AFB1 in edible oils.展开更多
This paper develops a semi-analytical solution for pile penetration in natural soft clays using the strain path method(SPM).The stress-strain behavior of soils is characterized by the S-CLAY1S model,which can capture ...This paper develops a semi-analytical solution for pile penetration in natural soft clays using the strain path method(SPM).The stress-strain behavior of soils is characterized by the S-CLAY1S model,which can capture the anisotropic evolution and destructuring nature of soft clays.By integrating the S-CLAY1S model into the theoretical framework of the SPM,a set of ordinary differential equations is formulated with respect to the vertical coordinate of soil particles.The distribution of excess pore water pressure(EPWP)following pile installation is approximated through one-dimensional(1D)radial integration around the pile shaft.The distribution of stresses and EPWP,along with the evolution of fabric anisotropy within the soil surrounding the pile,is presented to illustrate the response of pile penetration in natural soft clays.The proposed solution is validated against existing theoretical solutions using the SPM and cavity expansion method(CEM),along with experimental data.The findings demonstrate that the SPM reveals lower radial effective stresses and EPWP at the pile shaft than that of CEM.Pile penetration alters the soil's anisotropic properties,inducing rotational hardening and affecting post-installation stress distribution.Soil destructuration eliminates bonding among particles near the pile,resulting in a complete disruption of soil structure at the pile surface,which is particularly pronounced for higher initial soil structure ratios.Minimal variation was observed in the three principal stresses and shear stress on the cone side surface as the angle increased from 18°to 60°,except for a slight reduction in EPWP.展开更多
In this paper,a novel method for investigating the particle-crushing behavior of breeding particles in a fusion blanket is proposed.The fractal theory and Weibull distribution are combined to establish a theoretical m...In this paper,a novel method for investigating the particle-crushing behavior of breeding particles in a fusion blanket is proposed.The fractal theory and Weibull distribution are combined to establish a theoretical model,and its validity was verified using a simple impact test.A crushable discrete element method(DEM)framework is built based on the previously established theoretical model.The tensile strength,which considers the fractal theory,size effect,and Weibull variation,was assigned to each generated particle.The assigned strength is then used for crush detection by comparing it with its maximum tensile stress.Mass conservation is ensured by inserting a series of sub-particles whose total mass was equal to the quality loss.Based on the crushable DEM framework,a numerical simulation of the crushing behavior of a pebble bed with hollow cylindrical geometry under a uniaxial compression test was performed.The results of this investigation showed that the particle withstands the external load by contact and sliding at the beginning of the compression process,and the results confirmed that crushing can be considered an important method of resisting the increasing external load.A relatively regular particle arrangement aids in resisting the load and reduces the occurrence of particle crushing.However,a limit exists to the promotion of resistance.When the strain increases beyond this limit,the distribution of the crushing position tends to be isotropic over the entire pebble bed.The theoretical model and crushable DEM framework provide a new method for exploring the pebble bed in a fusion reactor,considering particle crushing.展开更多
Convex feasibility problems are widely used in image reconstruction, sparse signal recovery, and other areas. This paper is devoted to considering a class of convex feasibility problem arising from sparse signal recov...Convex feasibility problems are widely used in image reconstruction, sparse signal recovery, and other areas. This paper is devoted to considering a class of convex feasibility problem arising from sparse signal recovery. We first derive the projection formulas for a vector onto the feasible sets. The centralized circumcentered-reflection method is designed to solve the convex feasibility problem. Some numerical experiments demonstrate the feasibility and effectiveness of the proposed algorithm, showing superior performance compared to conventional alternating projection methods.展开更多
Marine thin plates are susceptible to welding deformation owing to their low structural stiffness.Therefore,the efficient and accurate prediction of welding deformation is essential for improving welding quality.The t...Marine thin plates are susceptible to welding deformation owing to their low structural stiffness.Therefore,the efficient and accurate prediction of welding deformation is essential for improving welding quality.The traditional thermal elastic-plastic finite element method(TEP-FEM)can accurately predict welding deformation.However,its efficiency is low because of the complex nonlinear transient computation,making it difficult to meet the needs of rapid engineering evaluation.To address this challenge,this study proposes an efficient prediction method for welding deformation in marine thin plate butt welds.This method is based on the coupled temperature gradient-thermal strain method(TG-TSM)that integrates inherent strain theory with a shell element finite element model.The proposed method first extracts the distribution pattern and characteristic value of welding-induced inherent strain through TEP-FEM analysis.This strain is then converted into the equivalent thermal load applied to the shell element model for rapid computation.The proposed method-particularly,the gradual temperature gradient-thermal strain method(GTG-TSM)-achieved improved computational efficiency and consistent precision.Furthermore,the proposed method required much less computation time than the traditional TEP-FEM.Thus,this study lays the foundation for future prediction of welding deformation in more complex marine thin plates.展开更多
To investigate the damage evolution caused by stress-driven and sub-critical crack propagation within the Beishan granite under multi-creep triaxial compressive conditions,the distributed optical fiber sensing and X-r...To investigate the damage evolution caused by stress-driven and sub-critical crack propagation within the Beishan granite under multi-creep triaxial compressive conditions,the distributed optical fiber sensing and X-ray computed tomography were combined to obtain the strain distribution over the sample surface and internal fractures of the samples.The Gini and skewness(G-S)coefficients were used to quantify strain localization during tests,where the Gini coefficient reflects the degree of clustering of elements with high strain values,i.e.,strain localization/delocalization.The strain localization-induced asymmetry of data distribution is quantified by the skewness coefficient.A precursor to granite failure is defined by the rapid and simultaneous increase of the G-S coefficients,which are calculated from strain increment,giving an earlier warning of failure by about 8%peak stress than those from absolute strain values.Moreover,the process of damage accumulation due to stress-driven crack propagation in Beishan granite is different at various confining pressures as the stress exceeds the crack initiation stress.Concretely,strain localization is continuous until brittle failure at higher confining pressure,while both strain localization and delocalization occur at lower confining pressure.Despite the different stress conditions,a similar statistical characteristic of strain localization during the creep stage is observed.The Gini coefficient increases,and the skewness coefficient decreases slightly as the creep stress is below 95%peak stress.When the accelerated strain localization begins,the Gini and skewness coefficients increase rapidly and simultaneously.展开更多
In this work,the Hierarchical Quadrature Element Method(HQEM)formulation of geometrically exact shells is proposed and applied for geometrically nonlinear analyses of both isotropic and laminated shells.The stress res...In this work,the Hierarchical Quadrature Element Method(HQEM)formulation of geometrically exact shells is proposed and applied for geometrically nonlinear analyses of both isotropic and laminated shells.The stress resultant formulation is developed within the HQEM framework,consequently significantly simplifying the computations of residual force and stiffness matrix.The present formulation inherently avoids shear and membrane locking,benefiting from its high-order approximation property.Furthermore,HQEM’s independent nodal distribution capability conveniently supports local p-refinement and flexibly facilitates mesh generation in various structural configurations through the combination of quadrilateral and triangular elements.Remarkably,in lateral buckling analysis,the HQEM outperforms the weak-form quadrilateral element(QEM)in accuracy with identical nodal degrees of freedom(three displacements and two rotations).Under high-load nonlinear response,the QEM exhibits a maximum relative deviation of approximately 9.5%from the reference,while the HQEM remains closely aligned with the benchmark results.In addition,for the cantilever beam under tip moment,HQEM produces virtually no out-of-plane deviation,compared to a slight deviation of 0.00001 with QEM,confirming its superior numerical reliability.In summary,the method demonstrates high accuracy,superior convergence,and robustness in handling large rotations and complex post-buckling behaviors across a series of benchmark problems.展开更多
Geological prospecting and the identification of adverse geological features are essential in tunnel construction,providing critical information to ensure safety and guide engineering decisions.As tunnel projects exte...Geological prospecting and the identification of adverse geological features are essential in tunnel construction,providing critical information to ensure safety and guide engineering decisions.As tunnel projects extend into deeper and more mountainous terrains,engineers face increasingly complex geological conditions,including high water pressure,intense geo-stress,elevated geothermal gradients,and active fault zones.These conditions pose substantial risks such as high-pressure water inrush,largescale collapses,and tunnel boring machine(TBM)blockages.Addressing these challenges requires advanced detection technologies capable of long-distance,high-precision,and intelligent assessments of adverse geology.This paper presents a comprehensive review of recent advancements in tunnel geological ahead prospecting methods.It summarizes the fundamental principles,technical maturity,key challenges,development trends,and real-world applications of various detection techniques.Airborne and semi-airborne geophysical methods enable large-scale reconnaissance for initial surveys in complex terrain.Tunnel-and borehole-based approaches offer high-resolution detection during excavation,including seismic ahead prospecting(SAP),TBM rock-breaking source seismic methods,fulltime-domain tunnel induced polarization(TIP),borehole electrical resistivity,and ground penetrating radar(GPR).To address scenarios involving multiple,coexisting adverse geologies,intelligent inversion and geological identification methods have been developed based on multi-source data fusion and artificial intelligence(AI)techniques.Overall,these advances significantly improve detection range,resolution,and geological characterization capabilities.The methods demonstrate strong adaptability to complex environments and provide reliable subsurface information,supporting safer and more efficient tunnel construction.展开更多
Stand age plays a crucial role in forest biomass estimation and carbon cycle modeling.Assessing the uncertainty of stand age prediction models and identifying the key driving factors in the modeling process have becom...Stand age plays a crucial role in forest biomass estimation and carbon cycle modeling.Assessing the uncertainty of stand age prediction models and identifying the key driving factors in the modeling process have become major challenges in forestry research.In this study,we selected the Shaanxi-Gansu-Ningxia region of Northeast China as the research area and utilized multi-source datasets from the summer of 2019 to extract information on spectral,textural,climatic,water balance,and stand characteristics.By integrating the Random Forest(RF)model with Monte Carlo(MC)simulation,we constructed six regression models based on different combina-tions of features and evaluated the uncertainty of each model.Furthermore,we investigated the driving factors influencing stand age modeling by analyzing the effects of different types of features on age inversion.Model performance and accuracy were assessed using the root mean square error(RMSE),mean absolute error(MAE),and the coefficient of determination(R^(2)),while the relative root mean square error(rRMSE)was employed to quantify model uncertainty.The results indicate that the scenarios with more obvious improve-ment in accuracy and effective reduction in uncertainty were Scenario 3 with the inclusion of climate and water balance information(RMSE=25.54 yr,MAE=18.03 yr,R^(2)=0.51,rRMSE=19.17%)and Scenario 5 with the inclusion of stand characterization informa-tion(RMSE=18.47 yr,MAE=13.05 yr,R^(2)=0.74,rRMSE=16.99%).Scenario 6,incorporating all feature types,achieved the highest accuracy(RMSE=17.60 yr,MAE=12.06 yr,R^(2)=0.77,rRMSE=14.19%).In this study,elevation,minimum temperature,and diameter at breast height(DBH)emerged as the key drivers of stand-age modeling.The proposed method can be used to identify drivers and to quantify uncertainty in stand-age estimation,providing a useful reference for improving model accuracy and uncertainty assessment.展开更多
Junctions are an important structure that allows charge separation in solar cells and photocatalysts. Here, we studied the charge transfer at an anatase/rutile TiO2 phase junction using time-resolved photoluminescence...Junctions are an important structure that allows charge separation in solar cells and photocatalysts. Here, we studied the charge transfer at an anatase/rutile TiO2 phase junction using time-resolved photoluminescence spectroscopy. Visible （-S00 nm） and near-infrared （NIR, -830 nm） emissions were monitored to give insight into the photoinduced charges of anatase and rutile in the junction, respectively, New fast photoluminescence decay components appeared in the visible emission of futile-phase dominated TiO2 and in the NIR emission of many mixed phase TiO2samples. The fast decays confirmed that the charge separation occurred at the phase junction. The visible emission intensity from the mixed phase TiO2 increased, revealing that charge transfer from rutile to anatase was the main pathway. The charge separation slowed the microsecond time scale photolumines- cence decay rate for charge carriers in both anatase and rutile. However, the millisecond decay of the charge carriers in anatase TiO2 was accelerated, while there was almost no change in the charge carrier dynamics of rutile TiO2. Thus, charge separation at the anatase/rutile phase junction caused an increase in the charge carrier concentration on a microsecond time scale, because of slower electron-hole recombination. The enhanced photocatalytic activity previously observed at ana- tase/rutile phase junctions is likely caused by the improved charge carrier dynamics we report here. These findings may contribute to the development of improved photocatalytic materials.展开更多
The ultrafast dynamics through conical intersections in 2,6-dimethylpyridine has been studied by femtosecond time-resolved photoelectron imaging coupled with time-resolved mass spectroscopy. Upon absorption of 266 nm ...The ultrafast dynamics through conical intersections in 2,6-dimethylpyridine has been studied by femtosecond time-resolved photoelectron imaging coupled with time-resolved mass spectroscopy. Upon absorption of 266 nm pump laser, 2,6-dimethylpyridine is excited to the S2 state with a ππ character from So state. The time evolution of the parent ion signals consists of two exponential decays. One is a fast component on a timescale of 635 fs and the other is a slow component with a timescale of 4.37 ps. Time-dependent photo- electron angular distributions and energy-resolved photoelectron spectroscopy are extracted from time-resolved photoelectron imaging and provide the evolutive information of S2 state. In brief, the ultrafast component is a population transfer from S2 to S1 through the S2/S1 conical intersections, the slow component is attributed to simultaneous IC from the S2 state and the higher vibrational levels of S1 state to So state, which involves the coupling of S2/S0 and S1/So conical intersections. Additionally, the observed ultrafast S2--＋S1 transition occurs only with an 18% branching ratio.展开更多
The function of protein in long-range biological electron transfer is a question of debate. We report some preliminary results in femtosecond spectroscopic study of photosynthetic bacterial light-harvesting antenna co...The function of protein in long-range biological electron transfer is a question of debate. We report some preliminary results in femtosecond spectroscopic study of photosynthetic bacterial light-harvesting antenna complex assembled onto TiO2 nanoparticle with an average size of 8 nm in diameter. Crystal structure shows that photosynthetic bacterial antenna complex LH2 has a ring-like structure composed by alpha- and beta-apoprotein helices. The alpha- and beta-transmembrance helices construct two concentric cylinders with pigments bacteriochlorophyll a (Bchl a) and carotenoid (Car) buried inside the protein. We attempt to insert TiO2 nanoparticle into the cavity of the inner cylindrical hollow of LH2 to investigate the nature of the electron transfer between the excited-state Bchl a and the TiO2 nanoparticle. A significant decrease in the ground state bleaching recovery time constant for Bchl a at 850 run (B850) in respect to that of the Bchl a in free LH2 has been observed. By using the relation of distance-dependent long-range electron transfer rate in protein, the distance between the donor B850 and the acceptor TiO2 nanoparticle has been estimated, which is about 0.6 nm. The proposed method of assembling proteins onto wide-gap semiconductor nanoparticle can be a promising way to determine the role of the protein playing in biological electron transfer processes.展开更多
基金Project supported by the National Natural Science Foundation of China(Grant No.62305087)。
文摘We performed a quantitative analysis of time-resolved laser-induced breakdown air plasma spectra to obtain the evolution of temperatures and species relative fractions.The air plasma was generated by focusing a 100 mJ Nd:YAG laser pulse,and the time-resolved spectra were recorded by an intensified charge-coupled device camera with incremental delay.The attention was mainly focused on the emission spectra of the first negative system of nitrogen(N_(2)^(+),B^(2)Σ-(u)^(-)-X^(2)Σ^(+)g)and the violet system of carbon nitride(CN,B^(2)Σ^(+)-X^(2)Σ^(+))located at 383-396 nm.A custom-built model was developed to perform the simulation and fitting of the N_(2)^(+)and the CN spectra from the air plasma.The model was verified by comparing to a published model with a 0.9860 Spearman correlation coefficient.With this model,the time-resolved non-equilibrium temperatures and relative fractions of N_(2)^(+)and CN were obtained with a fitting correlation coefficient higher than 0.9108.
基金financially supported by the National Key R&D Program of China(Nos.2023YFB3812400,2023YFB3812403)National Natural Foundation of China(Nos.52273206,52350233)+1 种基金Hunan Provincial Natural Science Foundation(No.2021JJ10029)Huxiang High-level Talent Gathering Project(No.2022RC4039).
文摘Photoswitchable fluorescent polymeric nanoparticles were widely concerned because of their excellent features including the flexible design,easy preparation and functionalization,and thus exhibited great application potential in information encryption,anti-counterfeiting,but remained challenging in improving the security.Herein,we described a self-erased time-resolved information encryption via using photoswitchable dual-color fluorescent polymeric nanoparticles(PDFPNs)containing two fluorescence dyes(blue and red)and photochromic spiroxazine derivatives.In view of the different thermo-induced isomerization rates of photochromic spiroxazine derivatives in different flexible substrates,the decoloration rate of PDFPNs can be programmatically tuned by regulating ratio between rigid polymer and flexible polymer.Therefore,after ultraviolet light(UV)irradiation,correct information could only be recognized in preestablished time during the self-erased process.Our results indicated that PDFPNs exhibited fast photo-responsibility(2 min),high fluorescence contrast,well-pleasing photo-reversibility(>20 times),and programmable thermo-responsiveness(24 s-6 h).We thus demonstrated their application in the selferased time-resolved information encryption and anti-counterfeiting with high security.
基金the National Key R&D Program of China(Grants Nos.2024YFA1408702 and 2021YFA1401903)Beijing Natural Science Foundation(Grant No.JQ24001)the National Natural Science Foundation of China(Grant No.12374143)。
文摘Quantum materials have attracted a great deal of attention because of their rich landscape of electronic structures,topological phases,strong correlation effects,and exotic orders.These systems provide a fertile platform for the exploration of novel quantum phenomena and materials applications.Particularly exciting is the exploration of nonequilibrium dynamics in quantum materials,which has significant research and potential application values.Pump-probe techniques play a key role in revealing the dynamics of quantum materials on remarkably short timescales,providing an attractive yet challenging avenue of research.In this context,time-resolved x-ray as an emerging probe exhibits high time resolution,momentum resolution,and substantial momentum coverage.It can reveal unprecedented transient states,distinguish between entangled ordered states,and has a compelling potential to probe ultrafast dynamics in a wide variety of quantum materials.Despite its unique advantages,time-resolved x-ray scattering still faces several technological and methodological challenges.In this review,we highlight recent advances focusing on the use of time-resolved x-ray scattering to probe dynamic processes in quantum materials.We discuss representative examples across structural,electronic,magnetic,and lattice degrees of freedom,and outline promising directions for future research in this rapidly evolving field.
基金the National Institute of Health for supporting this research under grants NIH R35GM152076,NIH 1SC1GM127175-01,NIH T32GM148394.
文摘Time-resolved flow cytometry(TRFC)was used to measure metabolic differences in estrogen receptor-positive breast cancer cells.This specialty cytometry technique measures fluorescence lifetimes as a single-cell parameter thereby providing a unique approach for high-throughput cell counting and screening.Differences in fluorescence lifetime were detected and this was associated with sensitivity to the commonly prescribed therapeutic tamoxifen.Differences in fluorescence lifetime are attributed to the binding states of the autofluorescent metabolite NAD(P)H.The function of NAD(P)H is well described and in general involves cycling from a reduced to oxidized state to facilitate electron transport for the conversion of pyruvate to lactate.NAD(P)H fluorescence lifetimes depend on the bound or unbound state of the metabolite,which also relates to metabolic transitions between oxidative phosphorylation and glycolysis.To determine if fundamental metabolic profiles differ for cells that are sensitive to tamoxifen compared to those that are resistant,large populations of MCF-7 breast cancer cells were screened and fluorescence lifetimes were quantified.Additionally,metabolic differences associated with tamoxifen sensitivity were measured with a Seahorse HS mini metabolic analyzer(Agilent Technologies Inc.Santa Clara,CA)and confocal imaging.Results show that tamoxifen-resistant breast cancer cells have increased utilization of glycolysis for energy production compared to tamoxifen-sensitive breast cancer cells.This work is impacting because it establishes an early step toward developing a reliable screening technology in which large cell censuses can be differentiated for drug sensitivity in a label-free fashion.
基金Supported in part by Natural Science Foundation of Guangxi(2023GXNSFAA026246)in part by the Central Government's Guide to Local Science and Technology Development Fund(GuikeZY23055044)in part by the National Natural Science Foundation of China(62363003)。
文摘In this paper,we consider the maximal positive definite solution of the nonlinear matrix equation.By using the idea of Algorithm 2.1 in ZHANG(2013),a new inversion-free method with a stepsize parameter is proposed to obtain the maximal positive definite solution of nonlinear matrix equation X+A^(*)X|^(-α)A=Q with the case 0<α≤1.Based on this method,a new iterative algorithm is developed,and its convergence proof is given.Finally,two numerical examples are provided to show the effectiveness of the proposed method.
基金supported by the Fuxing Nursing Research Foundation of Fudan University[FNF202352].
文摘Objectives This review aimed to systematically synthesize the available research on the disclosure of diagnosis and related issues in childhood cancer from the perspectives of healthcare professionals,with the goal of informing the optimization of disclosure processes and meeting the communication needs of affected families.Methods In accordance with the Joanna Briggs Institute(JBI)methodology for mixed methods systematic reviews,the convergent segregated approach was used in this review.Articles were retrieved from 11 databases,including PubMed,Web of Science,CINAHL,CENTRAL,Embase,Ovid/Medline,PsycINFO,PsycArticles,Scopus,ERIC,and China National Knowledge Infrastructure(CNKI).The quality of the selected articles was assessed using the Mixed Method Appraisal Tool(MMAT).The review protocol was registered on PROSPERO(CRD42024542746).Results A total of 21 studies from 10 countries were included.Their methodological quality was generally medium to high,with MMAT scores ranging from 60%to 100%.The synthesis yielded three core themes:1)the spectrum of professional and societal attitudes toward disclosure;2)the dynamic practices of navigating disclosure amid uncertainty,including timing and environment,stakeholders,and content of disclosure;and 3)factors influencing disclosure,including children’s,parental,healthcare professionals’,and socio-cultural factors.Conclusions This review synthesized the perspectives and experiences of healthcare professionals regarding disclosure in childhood cancer,highlighting the complexity and multidimensional nature of this process in clinical practice.Future research should further investigate the experiences and needs of children and their parents,explore cultural variations in disclosure practices,develop context-appropriate assessment tools,and construct multidimensional intervention strategies to enhance the humanistic care and professional effectiveness of the disclosure process.
基金supported by the National Natural Science Foundation of China(Grant Nos.12272393 and 52130905).
文摘As binary geological media,soil-rock mixtures(SRMs)exhibit a distinct gradational composition,leading to their unique mechanical behaviors.To appraise the stability of SRM slopes,it is essential to determine equivalent parameters of SRMs,which are typically obtained through experimental and numerical methods.In contrasted to other numerical methods,the numerical manifold method(NMM)is more effective in addressing SRM problems.This is because the high-precision regular mathematical meshes in NMM can be used without aligning with the soil-rock interfaces and boundaries of SRMs.In the current research,the equivalent strength parameters of SRMs,i.e.the equivalent cohesion ce and internal friction angleϕ_(e),are determined using NMM.Initially,an NMM triaxial numerical model is established and validated based on triaxial experiments.Subsequently,the soil and rock parameters are derived through parameter inversion.Moreover,the impacts of rock content,size,shape and rock blocks'major-axis orientation on ce andϕ_(e) of SRMs are thoroughly examined using the NMM triaxial numerical model.Additionally,a fitting function is proposed to linkϕ_(e) to the rock content and size of SRMs.When other influencing factors are fixed,the above fitting model leads to the following conclusions:(1)the predictedϕ_(e) of SRMs increase with the increase of rock content;and(2)SRM samples with smaller rocks display a higher predictedϕ_(e).
文摘The Good Wife is an American TV series that focuses on women’s independence,politics,and law.The drama has been remade in China,Japan,and South Korea.This research aims to use Nida’s Functional Equivalence Theory to analyze the methods of its English-to-Chinese subtitle translation by considering social,cultural,and historic backgrounds between China and America.After data collection and case analysis,the study found that:(1)Five major translation methods are adopted in the subtitle translation of The Good Wife.They are free translation,variation,literal translation,addition,and omission.Among them,free translation is the most frequently used,while omission is used least.(2)The subtitle translation of films and TV series is limited by time and space restrictions,social-cultural differences,and other factors.When translating,translators should try to use humorous words,euphemism,intonation,and other ways,and combine different methods such as literal translation,free translation,variation,addition,omission,and other methods to seek equivalence both in the meaning and function of subtitles under the guidance of Functional Equivalence Theory.
基金This work was supported by Special Fund for Grain -scientific Research in the Public Interest （201513006-02）, Special Fund for Agro -scientific Research in the Public Interest （201203094）, Natural Science Foundation of China （31401601）.
文摘Edible oil is one major nutritional ingredient to human and widely consumed directly. The contamination of aflatoxin B1 （AFB1） in edible oils has been attracted exten-sive efforts due to its hazard to human health and life. To avoid the digestion of edible oils contaminated by AFB1 the development of rapid and sensitive sensing method for AFB1 is required. Herein, a quantitative, sensitive and rapid method for AFB1 detection in edible oils was proposed by using ultrasensitive time-resolved fluorescent immunosensing （TRFIS） method. This method poses unique advantages from both time-resolved fluorescent sens-ing method and immunochromatographic assay format. The nanospheres were modified with fluorescent europium and then captured the home-made monoclonal antibody against AFB1 （3G1）. After optimization, by using a competitive immunosensing manner, this TRFIS method has a detectable linear range of 0.54-20.0 μg/kg with minimum detectable concen-tration of 0.18μg/kg. It can be completed merely within 10 min with recovery from 87.0% to 121.9%. The agreement was observed between the results by TRFIS and high perfor-mance liquid chromatography （HPLC） methods. This research provides a promising sens-ing method for sensitive and rapid determining AFB1 in edible oils.
基金support from the National Natural Science Foundation of China(Grant No.42407256)the State Key Laboratory of Hydraulics and Mountain River Engineering,China(Grant No.SKHL2113)the Sichuan Science and Technology Program(Grant No.2024YFHZ0341).
文摘This paper develops a semi-analytical solution for pile penetration in natural soft clays using the strain path method(SPM).The stress-strain behavior of soils is characterized by the S-CLAY1S model,which can capture the anisotropic evolution and destructuring nature of soft clays.By integrating the S-CLAY1S model into the theoretical framework of the SPM,a set of ordinary differential equations is formulated with respect to the vertical coordinate of soil particles.The distribution of excess pore water pressure(EPWP)following pile installation is approximated through one-dimensional(1D)radial integration around the pile shaft.The distribution of stresses and EPWP,along with the evolution of fabric anisotropy within the soil surrounding the pile,is presented to illustrate the response of pile penetration in natural soft clays.The proposed solution is validated against existing theoretical solutions using the SPM and cavity expansion method(CEM),along with experimental data.The findings demonstrate that the SPM reveals lower radial effective stresses and EPWP at the pile shaft than that of CEM.Pile penetration alters the soil's anisotropic properties,inducing rotational hardening and affecting post-installation stress distribution.Soil destructuration eliminates bonding among particles near the pile,resulting in a complete disruption of soil structure at the pile surface,which is particularly pronounced for higher initial soil structure ratios.Minimal variation was observed in the three principal stresses and shear stress on the cone side surface as the angle increased from 18°to 60°,except for a slight reduction in EPWP.
基金supported by Anhui Provincial Natural Science Foundation(2408085QA030)Natural Science Research Project of Anhui Educational Committee,China(2022AH050825)+3 种基金Medical Special Cultivation Project of Anhui University of Science and Technology(YZ2023H2C008)the Excellent Research and Innovation Team of Anhui Province,China(2022AH010052)the Scientific Research Foundation for High-level Talents of Anhui University of Science and Technology,China(2021yjrc51)Collaborative Innovation Program of Hefei Science Center,CAS,China(2019HSC-CIP006).
文摘In this paper,a novel method for investigating the particle-crushing behavior of breeding particles in a fusion blanket is proposed.The fractal theory and Weibull distribution are combined to establish a theoretical model,and its validity was verified using a simple impact test.A crushable discrete element method(DEM)framework is built based on the previously established theoretical model.The tensile strength,which considers the fractal theory,size effect,and Weibull variation,was assigned to each generated particle.The assigned strength is then used for crush detection by comparing it with its maximum tensile stress.Mass conservation is ensured by inserting a series of sub-particles whose total mass was equal to the quality loss.Based on the crushable DEM framework,a numerical simulation of the crushing behavior of a pebble bed with hollow cylindrical geometry under a uniaxial compression test was performed.The results of this investigation showed that the particle withstands the external load by contact and sliding at the beginning of the compression process,and the results confirmed that crushing can be considered an important method of resisting the increasing external load.A relatively regular particle arrangement aids in resisting the load and reduces the occurrence of particle crushing.However,a limit exists to the promotion of resistance.When the strain increases beyond this limit,the distribution of the crushing position tends to be isotropic over the entire pebble bed.The theoretical model and crushable DEM framework provide a new method for exploring the pebble bed in a fusion reactor,considering particle crushing.
基金Supported by the Natural Science Foundation of Guangxi Province(Grant Nos.2023GXNSFAA026067,2024GXN SFAA010521)the National Natural Science Foundation of China(Nos.12361079,12201149,12261026).
文摘Convex feasibility problems are widely used in image reconstruction, sparse signal recovery, and other areas. This paper is devoted to considering a class of convex feasibility problem arising from sparse signal recovery. We first derive the projection formulas for a vector onto the feasible sets. The centralized circumcentered-reflection method is designed to solve the convex feasibility problem. Some numerical experiments demonstrate the feasibility and effectiveness of the proposed algorithm, showing superior performance compared to conventional alternating projection methods.
基金Supported by the National Natural Science Foundation of China under Grant No.51975138the High-Tech Ship Scientific Research Project from the Ministry of Industry and Information Technology under Grant No.CJ05N20the National Defense Basic Research Project under Grant No.JCKY2023604C006.
文摘Marine thin plates are susceptible to welding deformation owing to their low structural stiffness.Therefore,the efficient and accurate prediction of welding deformation is essential for improving welding quality.The traditional thermal elastic-plastic finite element method(TEP-FEM)can accurately predict welding deformation.However,its efficiency is low because of the complex nonlinear transient computation,making it difficult to meet the needs of rapid engineering evaluation.To address this challenge,this study proposes an efficient prediction method for welding deformation in marine thin plate butt welds.This method is based on the coupled temperature gradient-thermal strain method(TG-TSM)that integrates inherent strain theory with a shell element finite element model.The proposed method first extracts the distribution pattern and characteristic value of welding-induced inherent strain through TEP-FEM analysis.This strain is then converted into the equivalent thermal load applied to the shell element model for rapid computation.The proposed method-particularly,the gradual temperature gradient-thermal strain method(GTG-TSM)-achieved improved computational efficiency and consistent precision.Furthermore,the proposed method required much less computation time than the traditional TEP-FEM.Thus,this study lays the foundation for future prediction of welding deformation in more complex marine thin plates.
基金supported by the National Natural Science Foundation of China(Grant No.52339001).
文摘To investigate the damage evolution caused by stress-driven and sub-critical crack propagation within the Beishan granite under multi-creep triaxial compressive conditions,the distributed optical fiber sensing and X-ray computed tomography were combined to obtain the strain distribution over the sample surface and internal fractures of the samples.The Gini and skewness(G-S)coefficients were used to quantify strain localization during tests,where the Gini coefficient reflects the degree of clustering of elements with high strain values,i.e.,strain localization/delocalization.The strain localization-induced asymmetry of data distribution is quantified by the skewness coefficient.A precursor to granite failure is defined by the rapid and simultaneous increase of the G-S coefficients,which are calculated from strain increment,giving an earlier warning of failure by about 8%peak stress than those from absolute strain values.Moreover,the process of damage accumulation due to stress-driven crack propagation in Beishan granite is different at various confining pressures as the stress exceeds the crack initiation stress.Concretely,strain localization is continuous until brittle failure at higher confining pressure,while both strain localization and delocalization occur at lower confining pressure.Despite the different stress conditions,a similar statistical characteristic of strain localization during the creep stage is observed.The Gini coefficient increases,and the skewness coefficient decreases slightly as the creep stress is below 95%peak stress.When the accelerated strain localization begins,the Gini and skewness coefficients increase rapidly and simultaneously.
基金supported by the National Natural Science Foundation of China(Grant Nos.12472194,12002018,11972004,11772031,11402015).
文摘In this work,the Hierarchical Quadrature Element Method(HQEM)formulation of geometrically exact shells is proposed and applied for geometrically nonlinear analyses of both isotropic and laminated shells.The stress resultant formulation is developed within the HQEM framework,consequently significantly simplifying the computations of residual force and stiffness matrix.The present formulation inherently avoids shear and membrane locking,benefiting from its high-order approximation property.Furthermore,HQEM’s independent nodal distribution capability conveniently supports local p-refinement and flexibly facilitates mesh generation in various structural configurations through the combination of quadrilateral and triangular elements.Remarkably,in lateral buckling analysis,the HQEM outperforms the weak-form quadrilateral element(QEM)in accuracy with identical nodal degrees of freedom(three displacements and two rotations).Under high-load nonlinear response,the QEM exhibits a maximum relative deviation of approximately 9.5%from the reference,while the HQEM remains closely aligned with the benchmark results.In addition,for the cantilever beam under tip moment,HQEM produces virtually no out-of-plane deviation,compared to a slight deviation of 0.00001 with QEM,confirming its superior numerical reliability.In summary,the method demonstrates high accuracy,superior convergence,and robustness in handling large rotations and complex post-buckling behaviors across a series of benchmark problems.
基金supported by the National Natural Science Foundation of China(Grant Nos.52021005,52325904,and 51991391)。
文摘Geological prospecting and the identification of adverse geological features are essential in tunnel construction,providing critical information to ensure safety and guide engineering decisions.As tunnel projects extend into deeper and more mountainous terrains,engineers face increasingly complex geological conditions,including high water pressure,intense geo-stress,elevated geothermal gradients,and active fault zones.These conditions pose substantial risks such as high-pressure water inrush,largescale collapses,and tunnel boring machine(TBM)blockages.Addressing these challenges requires advanced detection technologies capable of long-distance,high-precision,and intelligent assessments of adverse geology.This paper presents a comprehensive review of recent advancements in tunnel geological ahead prospecting methods.It summarizes the fundamental principles,technical maturity,key challenges,development trends,and real-world applications of various detection techniques.Airborne and semi-airborne geophysical methods enable large-scale reconnaissance for initial surveys in complex terrain.Tunnel-and borehole-based approaches offer high-resolution detection during excavation,including seismic ahead prospecting(SAP),TBM rock-breaking source seismic methods,fulltime-domain tunnel induced polarization(TIP),borehole electrical resistivity,and ground penetrating radar(GPR).To address scenarios involving multiple,coexisting adverse geologies,intelligent inversion and geological identification methods have been developed based on multi-source data fusion and artificial intelligence(AI)techniques.Overall,these advances significantly improve detection range,resolution,and geological characterization capabilities.The methods demonstrate strong adaptability to complex environments and provide reliable subsurface information,supporting safer and more efficient tunnel construction.
基金Under the auspices of the Natural Science Foundation of China(No.32371875,32001249)。
文摘Stand age plays a crucial role in forest biomass estimation and carbon cycle modeling.Assessing the uncertainty of stand age prediction models and identifying the key driving factors in the modeling process have become major challenges in forestry research.In this study,we selected the Shaanxi-Gansu-Ningxia region of Northeast China as the research area and utilized multi-source datasets from the summer of 2019 to extract information on spectral,textural,climatic,water balance,and stand characteristics.By integrating the Random Forest(RF)model with Monte Carlo(MC)simulation,we constructed six regression models based on different combina-tions of features and evaluated the uncertainty of each model.Furthermore,we investigated the driving factors influencing stand age modeling by analyzing the effects of different types of features on age inversion.Model performance and accuracy were assessed using the root mean square error(RMSE),mean absolute error(MAE),and the coefficient of determination(R^(2)),while the relative root mean square error(rRMSE)was employed to quantify model uncertainty.The results indicate that the scenarios with more obvious improve-ment in accuracy and effective reduction in uncertainty were Scenario 3 with the inclusion of climate and water balance information(RMSE=25.54 yr,MAE=18.03 yr,R^(2)=0.51,rRMSE=19.17%)and Scenario 5 with the inclusion of stand characterization informa-tion(RMSE=18.47 yr,MAE=13.05 yr,R^(2)=0.74,rRMSE=16.99%).Scenario 6,incorporating all feature types,achieved the highest accuracy(RMSE=17.60 yr,MAE=12.06 yr,R^(2)=0.77,rRMSE=14.19%).In this study,elevation,minimum temperature,and diameter at breast height(DBH)emerged as the key drivers of stand-age modeling.The proposed method can be used to identify drivers and to quantify uncertainty in stand-age estimation,providing a useful reference for improving model accuracy and uncertainty assessment.
基金supported by the National Natural Science Foundation of China (21203185, 21373209)the National Basic Research Program of China (2014CB239400)
文摘Junctions are an important structure that allows charge separation in solar cells and photocatalysts. Here, we studied the charge transfer at an anatase/rutile TiO2 phase junction using time-resolved photoluminescence spectroscopy. Visible （-S00 nm） and near-infrared （NIR, -830 nm） emissions were monitored to give insight into the photoinduced charges of anatase and rutile in the junction, respectively, New fast photoluminescence decay components appeared in the visible emission of futile-phase dominated TiO2 and in the NIR emission of many mixed phase TiO2samples. The fast decays confirmed that the charge separation occurred at the phase junction. The visible emission intensity from the mixed phase TiO2 increased, revealing that charge transfer from rutile to anatase was the main pathway. The charge separation slowed the microsecond time scale photolumines- cence decay rate for charge carriers in both anatase and rutile. However, the millisecond decay of the charge carriers in anatase TiO2 was accelerated, while there was almost no change in the charge carrier dynamics of rutile TiO2. Thus, charge separation at the anatase/rutile phase junction caused an increase in the charge carrier concentration on a microsecond time scale, because of slower electron-hole recombination. The enhanced photocatalytic activity previously observed at ana- tase/rutile phase junctions is likely caused by the improved charge carrier dynamics we report here. These findings may contribute to the development of improved photocatalytic materials.
基金This work was supported by the National Natural Science Foundation of China （No.10704083）,the Innovation Foundation of Chinese Academyof Sciences （No.KJCX1-YW-N30）, and the Public Science and Technology Program of Shenzhen （No.SY200806260026A）.
文摘The ultrafast dynamics through conical intersections in 2,6-dimethylpyridine has been studied by femtosecond time-resolved photoelectron imaging coupled with time-resolved mass spectroscopy. Upon absorption of 266 nm pump laser, 2,6-dimethylpyridine is excited to the S2 state with a ππ character from So state. The time evolution of the parent ion signals consists of two exponential decays. One is a fast component on a timescale of 635 fs and the other is a slow component with a timescale of 4.37 ps. Time-dependent photo- electron angular distributions and energy-resolved photoelectron spectroscopy are extracted from time-resolved photoelectron imaging and provide the evolutive information of S2 state. In brief, the ultrafast component is a population transfer from S2 to S1 through the S2/S1 conical intersections, the slow component is attributed to simultaneous IC from the S2 state and the higher vibrational levels of S1 state to So state, which involves the coupling of S2/S0 and S1/So conical intersections. Additionally, the observed ultrafast S2--＋S1 transition occurs only with an 18% branching ratio.
文摘The function of protein in long-range biological electron transfer is a question of debate. We report some preliminary results in femtosecond spectroscopic study of photosynthetic bacterial light-harvesting antenna complex assembled onto TiO2 nanoparticle with an average size of 8 nm in diameter. Crystal structure shows that photosynthetic bacterial antenna complex LH2 has a ring-like structure composed by alpha- and beta-apoprotein helices. The alpha- and beta-transmembrance helices construct two concentric cylinders with pigments bacteriochlorophyll a (Bchl a) and carotenoid (Car) buried inside the protein. We attempt to insert TiO2 nanoparticle into the cavity of the inner cylindrical hollow of LH2 to investigate the nature of the electron transfer between the excited-state Bchl a and the TiO2 nanoparticle. A significant decrease in the ground state bleaching recovery time constant for Bchl a at 850 run (B850) in respect to that of the Bchl a in free LH2 has been observed. By using the relation of distance-dependent long-range electron transfer rate in protein, the distance between the donor B850 and the acceptor TiO2 nanoparticle has been estimated, which is about 0.6 nm. The proposed method of assembling proteins onto wide-gap semiconductor nanoparticle can be a promising way to determine the role of the protein playing in biological electron transfer processes.
