Traditional linear vibration isolators struggle to combine high load-bearing capacity with low-frequency vibration isolation, whereas nonlinear metastructure isolators can effectively fulfill both functions. This pape...Traditional linear vibration isolators struggle to combine high load-bearing capacity with low-frequency vibration isolation, whereas nonlinear metastructure isolators can effectively fulfill both functions. This paper draws inspiration from the Quasi-Zero Stiffness (QZS) characteristics resulting from the buckling deformation of beams, and proposes a gear-based QZS structure by arranging beams in a circular array. We investigated the static mechanical behavior under different structural parameters, loading angles, and gear combinations through experiments and simulations, and demonstrated the mechanical performances could be effectively programmed. Subsequent vibration isolation tests on the double gears prove superior vibration isolation performance at low frequency while maintaining high load-bearing capacities. Additionally, a key contribution of our work is the development of a mathematical model to characterize the buckling behavior of the unit beam within the gear structure, with its accuracy validated through finite element analysis and experimental results. The gear’s modulus, number of teeth, and pressure angle are selected according to standard series, allowing the gear can be seamlessly integrated into existing mechanical systems in critical fields such as aerospace, military, and etc.展开更多
Photodetectors with long detection distances and fast response are important media in constructing a non-contact human-machine interface for the Masterly Internet of Things(MIT).All-inorganic perovskites have excellen...Photodetectors with long detection distances and fast response are important media in constructing a non-contact human-machine interface for the Masterly Internet of Things(MIT).All-inorganic perovskites have excellent optoelectronic performance with high moisture and oxygen resistance,making them one of the promising candidates for high-performance photodetectors,but a simple,low-cost and reliable fabrication technology is urgently needed.Here,a dual-function laser etching method is developed to complete both the lyophilic split-ring structure and electrode patterning.This novel split-ring structure can capture the perovskite precursor droplet efficiently and achieve the uniform and compact deposition of CsPbBr3 films.Furthermore,our devices based on laterally conducting split-ring structured photodetectors possess outstanding performance,including the maximum responsivity of 1.44×105 mA W^(−1),a response time of 150μs in 1.5 kHz and one-unit area<4×10-2 mm2.Based on these split-ring photodetector arrays,we realized three-dimensional gesture detection with up to 100 mm distance detection and up to 600 mm s^(−1) speed detection,for low-cost,integrative,and non-contact human-machine interfaces.Finally,we applied this MIT to wearable and flexible digital gesture recognition watch panel,safe and comfortable central controller integrated on the car screen,and remote control of the robot,demonstrating the broad potential applications.展开更多
With plenty of popular and effective ternary organic solar cells(OSCs)construction strategies proposed and applied,its power conversion efficiencies(PCEs)have come to a new level of over 19%in single-junction devices....With plenty of popular and effective ternary organic solar cells(OSCs)construction strategies proposed and applied,its power conversion efficiencies(PCEs)have come to a new level of over 19%in single-junction devices.However,previous studies are heavily based in chloroform(CF)leaving behind substantial knowledge deficiencies in understanding the influence of solvent choice when introducing a third component.Herein,we present a case where a newly designed asymmetric small molecular acceptor using fluoro-methoxylated end-group modification strategy,named BTP-BO-3FO with enlarged bandgap,brings different morphological evolution and performance improvement effect on host system PM6:BTP-eC9,processed by CF and ortho-xylene(o-XY).With detailed analyses supported by a series of experiments,the best PCE of 19.24%for green solvent-processed OSCs is found to be a fruit of finely tuned crystalline ordering and general aggregation motif,which furthermore nourishes a favorable charge generation and recombination behavior.Likewise,over 19%PCE can be achieved by replacing spin-coating with blade coating for active layer deposition.This work focuses on understanding the commonly met yet frequently ignored issues when building ternary blends to demonstrate cutting-edge device performance,hence,will be instructive to other ternary OSC works in the future.展开更多
Power-conversion-efficiencies(PCEs)of organic solar cells(OSCs)in laboratory,normally processed by spin-coating technology with toxic halogenated solvents,have reached over 19%.However,there is usually a marked PCE dr...Power-conversion-efficiencies(PCEs)of organic solar cells(OSCs)in laboratory,normally processed by spin-coating technology with toxic halogenated solvents,have reached over 19%.However,there is usually a marked PCE drop when the bladecoating and/or green-solvents toward large-scale printing are used instead,which hampers the practical development of OSCs.Here,a new series of N-alkyl-tailored small molecule acceptors named YR-SeNF with a same molecular main backbone are developed by combining selenium-fused central-core and naphthalene-fused endgroup.Thanks to the N-alkyl engineering,NIR-absorbing YR-SeNF series show different crystallinity,packing patterns,and miscibility with polymeric donor.The studies exhibit that the molecular packing,crystallinity,and vertical distribution of active layer morphologies are well optimized by introducing newly designed vip acceptor associated with tailored N-alkyl chains,providing the improved charge transfer dynamics and stability for the PM6:L8-BO:YRSeNF-based OSCs.As a result,a record-high PCE approaching 19%is achieved in the blade-coating OSCs fabricated from a greensolvent o-xylene with high-boiling point.Notably,ternary OSCs offer robust operating stability under maximum-power-point tracking and well-keep>80%of the initial PCEs for even over 400 h.Our alkyl-tailored vip acceptor strategy provides a unique approach to develop green-solvent and blade-coating processed high-efficiency and operating stable OSCs,which paves a way for industrial development.展开更多
Lithium metal batteries(LMBs)are considered the ideal choice for high volumetric energy density lithium-ion batteries,but uncontrolled lithium deposition poses a significant challenge to the stability of such devices....Lithium metal batteries(LMBs)are considered the ideal choice for high volumetric energy density lithium-ion batteries,but uncontrolled lithium deposition poses a significant challenge to the stability of such devices.In this paper,we introduce a 2.5μm-thick asymmetric and ultrastrong separator,which can induce tissue-like lithium deposits.The asymmetric separator,denoted by utPE@Cu_(2)O,was prepared by selective synthesis of Cu_(2)O nanoparticles on one of the outer surfaces of a nanofibrous(diameter~10 nm)ultrastrong ultrahigh molecular weight polyethylene(UHMWPE)membrane.Microscopic analysis shows that the lithium deposits have tissue-like morphology,resulting in the symmetric lithium cells assembled using utPE@Cu_(2)O with symmetric Cu_(2)O coating exhibiting stable performance for over 2000 h of cycling.This work demonstrates the feasibility of a facile approach ultrathin separators for the deployment of lithium metal batteries,providing a pathway towards enhanced battery performance and safety.展开更多
Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of urea.Herein,we report copper carbonate hydroxide(Cu_2(OH)...Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of urea.Herein,we report copper carbonate hydroxide(Cu_2(OH)_2CO_(3))as an efficient CO_(2)NO_(3)RR electrocatalyst with an impressive urea Faradaic efficiency of45.2%±2.1%and a high yield rate of 1564.5±145.2μg h~(-1)mg_(cat)~(-1).More importantly,H_(2) evolution is fully inhibited on this electrocatalyst over a wide potential range between-0.3 and-0.8 V versus reversible hydrogen electrode.Our thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu_2(OH)_2CO_(3) by combining the two intermediates,~*COOH and~*NHO.This work demonstrates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO_(2)NO_(3)RR,and provide guidance for rational design of more advanced catalysts.展开更多
Transmutation is an efficient approach for material design. For example, ternary compound CuGaSe_(2) in chalcopyrite structure is a promising material for novel optoelectronic and thermoelectric device applications. I...Transmutation is an efficient approach for material design. For example, ternary compound CuGaSe_(2) in chalcopyrite structure is a promising material for novel optoelectronic and thermoelectric device applications. It can be considered as formed from the binary host compound ZnSe in zinc-blende structure by cation transmutation(i.e., replacing two Zn atoms by one Cu and one Ga). While cation-transmutated materials are common, aniontransmutated ternary materials are rare, for example, Zn_(2)As Br(i.e., replacing two Se atoms by one As and one Br)is not reported. The physical origin for this puzzling disparity is unclear. In this work, we employ first-principles calculations to address this issue, and find that the distinct differences in stability between cation-transmutated(mix-cation) and anion-transmutated(mix-anion) compounds originate from their different trends of ionic radii as functions of their ionic state, i.e., for cations, the radius decreases with the increasing ionic state, whereas for anions, the radius increases with the increasing absolute ionic state. Therefore, for mix-cation compounds,the strain energy and Coulomb energy can be simultaneously optimized to make these materials stable. In contrast, for mix-anion systems, minimization of Coulomb energy will increase the strain energy, thus the system becomes unstable or less stable. Thus, the trend of decreasing strain energy and Coulomb energy is consistent in mix-cation compounds, while it is opposite in mix-anion compounds. Furthermore, the study suggests that the stability strategy for mix-anion compounds can be controlled by the ratio of ionic radii r3/r1, with a smaller ratio indicating greater stability. Our work, thus, elucidates the intrinsic stability trend of transmutated materials and provides guidelines for the design of novel ternary materials for various device applications.展开更多
Semitransparent organic photovoltaics(STOPVs)have gained wide attention owing to their promising applications in building-integrated photovoltaics,agrivoltaics,and floating photovoltaics.Organic semiconductors with hi...Semitransparent organic photovoltaics(STOPVs)have gained wide attention owing to their promising applications in building-integrated photovoltaics,agrivoltaics,and floating photovoltaics.Organic semiconductors with high charge carrier mobility usually have planar and conjugated structures,thereby showing strong absorption in visible region.In this work,a new concept of incorporating transparent inorganic semiconductors is proposed for high-performance STOPVs.Copper(I)thiocyanate(CuSCN)is a visible-transparent inorganic semiconductor with an ionization potential of 5.45 eV and high hole mobility.The transparency of CuSCN benefits high average visible transmittance(AVT)of STOPVs.The energy levels of CuSCN as donor match those of near-infrared small molecule acceptor BTP-eC9,and the formed heterojunction exhibits an ability of exciton dissociation.High mobility of CuSCN contributes to a more favorable charge transport channel and suppresses charge recombination.The control STOPVs based on PM6/BTP-eC9 exhibit an AVT of 19.0%with a power conversion efficiency(PCE)of 12.7%.Partial replacement of PM6 with CuSCN leads to a 63%increase in transmittance,resulting in a higher AVT of 30.9%and a comparable PCE of 10.8%.展开更多
G-quartet(G4)-based circularly polarized luminescence(CPL)materials within CPL engineering have attracted substantial attention in optoelectronics and photonics owing to their excellent chiral properties and promising...G-quartet(G4)-based circularly polarized luminescence(CPL)materials within CPL engineering have attracted substantial attention in optoelectronics and photonics owing to their excellent chiral properties and promising applications in advanced optical devices.However,their practical use is limited by relatively low quantum yield(QY),which reduces emission efficiency.Addressing this challenge,we present BgoFace,an integrated active learning(AL)-based software,to optimize G4-based CPL materials with high QY.Starting with an initial dataset of 54 experimentally validated samples,the system executed six AL cycles encompassing 24 targeted experimental groups.Through this closed-loop workflow,BgoFace successfully identified G4 complexes exhibiting a near doubling of QY(37.25%).This achievement significantly advances the previously low QY values typically reported for G4-based CPL materials.The optimized materials demonstrate enhanced stability and processability,attributable to the AL algorithm's simultaneous consideration of multiple physicochemical parameters.This study not only advances the field of G4-based CPL materials for optical and photonic applications,but also establishes a generalizable AL framework suitable for optimizing functional nanomaterials in optoelectronic device design.By bridging datadriven design and experimental validation,BgoFace offers a transformative strategy for accelerating the development of functional nanomaterial engineering.展开更多
Fully non-fused electron acceptors(FNEAs)exhibit great potential as cost-effective electron acceptors for organic solar cells(OSCs).However,the device performance of FNEAs in OSCs is hindered by weak acceptor crystall...Fully non-fused electron acceptors(FNEAs)exhibit great potential as cost-effective electron acceptors for organic solar cells(OSCs).However,the device performance of FNEAs in OSCs is hindered by weak acceptor crystallinity associated with the rotation of carbon-carbon single bonds.Herein,we report the formation of strong molecular crystallinity of FNEAs and thus favorable fibril network morphology in blend films by finely optimizing the thermal annealing temperature.This favorable morphology not only enhanced the diffusion distance and dissociation efficiency of excitons in the acceptor phase,but also significantly boosted the electron mobility and carrier extraction rate.Consequently,a power conversion efficiency of 17.3%along with a short-circuit current density of 27.7 mA cm^(-2)are obtained,which are both the highest values for OSCs employing fully non-fused electron acceptors.These results demonstrate promising prospects and provide valuable insights for achieving high-efficiency OSCs using low-cost FNEAs.展开更多
The development of power conversion efficiency(PCE)for organic solar cells(OSCs)based on polymer donors with benzo[1,2-b:4,5-b′]-difuran building block is slower than that of those based on benzodithiophene due to un...The development of power conversion efficiency(PCE)for organic solar cells(OSCs)based on polymer donors with benzo[1,2-b:4,5-b′]-difuran building block is slower than that of those based on benzodithiophene due to uncontrollable aggregation behavior.However,the former is expected to be more promising in realizing environmentally friendly and high-performance devices.Thereby,a smart aggregation tuning strategy is needed for boosting the efficiency of this type of OSCs.Here we report solid additives designed by self-imitation strategy,which aims to control the aggregation of the donor D18-Fu,and regulate the domain expansion of the acceptor L8-BO.Three oligomeric additives,with or without halogenation,can uniformly reduce the energy loss and enhance charge generation compared to an additive-free control device.This improvement is demonstrated through a series of morphological characterizations,photophysical analyses and theoretical simulations,indicating strong interaction between additive molecules and donor&acceptor.As a result,a 19%PCE is reported in binary OSCs,which also represents the highest level for devices based on benzo[1,2-b:4,5-b′]-difuran core contained polymer donor.Apart from high performance,our study provides new insights into manipulating the competition between the donor and acceptor's pure phase formation through new additive design methods.展开更多
In this paper,an alkyl-chain-linked strategy is employed to synthesize a dimeric acceptor,DPhC8Y,which achieves simultaneous enhancements in device efficiency and stability while also exhibiting an unprecedentedly hig...In this paper,an alkyl-chain-linked strategy is employed to synthesize a dimeric acceptor,DPhC8Y,which achieves simultaneous enhancements in device efficiency and stability while also exhibiting an unprecedentedly high production yield compared to other“giant molecular acceptors”for organic solar cells(OSCs).Compared to the monomer DTY6,DPhC8Y contains improved crystalline ordering and refined phase separation,thereby reducing non-radiative loss,suppressing bulk and interface recombination,and decreasing trap density.On the other hand,the dimer acceptor possesses an intrinsically higher glass transition point.Through performance evaluation,the binary device of D18:DPhC8Y blend demonstrates 19.50%efficiency with remarkably over 80%fill factor(FF),surpassing those of D18:DTY6(18.25%and 76.42%).Meanwhile,the dimer-based active layer displays significantly enhanced storage and thermal stability in the device.Our report showcases the possibility of achieving OSCs with concurrent decent efficiency,stability,and cost-effectiveness through smart material and synthesis design.展开更多
Accelerating the discovery of advanced materials is crucial for modern industries,aerospace,biomedicine,and energy.Nevertheless,only a small fraction of materials are currently under experimental investigation within ...Accelerating the discovery of advanced materials is crucial for modern industries,aerospace,biomedicine,and energy.Nevertheless,only a small fraction of materials are currently under experimental investigation within the vast chemical space.Materials scientists are plagued by timeconsuming and labor-intensive experiments due to lacking efficient material discovery strategies.Artificial intelligence(AI)has emerged as a promising instrument to bridge this gap.Although numerous AI toolkits or platforms for material science have been developed,they suffer from many shortcomings.These include primarily focusing on material property prediction and being unfriendly to material scientists lacking programming experience,especially performing poorly with limited data.Here,we developed MLMD,an AI platformfor materials design.It is capable of effectively discovering novel materials with high-potential advanced properties end-to-end,utilizing model inference,surrogate optimization,and even working in situations of data scarcity based on active learning.Additionally,it integrates data analysis,descriptor refactoring,hyper-parameters auto-optimizing,and properties prediction.It also provides a web-based friendly interface without need programming and can be used anywhere,anytime.MLMD is dedicated to the integration of material experiment/computation and design,and accelerate the new material discovery with desired one or multiple properties.It demonstrates the strong power to direct experiments on various materials(perovskites,steel,high-entropy alloy,etc).MLMD will be an essential tool for materials scientists and facilitate the advancement of materials informatics.展开更多
The present study introduces a tribological comparison of five polyvinyl alcohol(PVA)hydrogel specimens with different physiological properties and possible candidate materials for cartilage replacement.The superior l...The present study introduces a tribological comparison of five polyvinyl alcohol(PVA)hydrogel specimens with different physiological properties and possible candidate materials for cartilage replacement.The superior lubrication of articular cartilage is believed to lie in solid-to-solid molecular interactions.Therefore,the focus was paid to the investigation of boundary lubrication with regard to interstitial fluid flow reduction.The experiments were carried out in a ball-on-plate(glass-on-hydrogel)configuration.Based on the experiments,we proposed a boundary lubrication mechanism,selected a hydrogel with the least surface damage,and highlighted the desired properties that should be considered when developing the artificial cartilage.展开更多
We present a multi-objective Bayesian active learning strategy,which greatly accelerates the discovery of super high-strength and high-ductility lead-free solder alloys.The active learning strategy demonstrates that a...We present a multi-objective Bayesian active learning strategy,which greatly accelerates the discovery of super high-strength and high-ductility lead-free solder alloys.The active learning strategy demonstrates that a machine learning model will have high generalizability if experimental data uncertainty is included,which greatly improves the model prediction or the material design accuracy.The feature-point-start forward method in multi-objective optimization adopts two Gaussian process regression(GPR)models,one for strength and one for elongation,and their outputs build up the acquisition-function-modified objective space of strength and elongation.Then,Bayesian sampling is applied to design the next experiments by balancing exploitation and exploration.Seven multi-objective active learning iterations discovered two novel super high-strength and high-ductility lead-free solder alloys.After that,various material characterizations were conducted on the two novel solder alloys,and the results exhibited their high performances in melting properties,wettability,electrical conductivity,and shear strength of the solder joint and explored the mechanism of high strength and high ductility of the alloys.The present work systematically analyzes the important role of experimental uncertainty in machine learning,especially in the global optimization for material design,which demands high generalizability of predictions.展开更多
The A-D-A and A-D-A'-D-A molecular skeletons of nonfullerene acceptors(NFAs)establish the success in realizing high-efficiency organic photovoltaics(OPVs),while the C=C bond between D and A moieties stands as a cr...The A-D-A and A-D-A'-D-A molecular skeletons of nonfullerene acceptors(NFAs)establish the success in realizing high-efficiency organic photovoltaics(OPVs),while the C=C bond between D and A moieties stands as a critical weakness for long-term stability.Herein,we report that by developing trichlorinated cyanoindone as A terminal,the resulting NFA denoted S-5Cl could resist both photodegradation with an increased rotational energy barrier and thermo-diffusion with the elevated glass transition temperature,which was further supported by tighter molecular stacking in the single crystal of S-5Cl.These features,thus,allow the S-5Cl-based binary OPV to possess 2–4 times longer lifetimes under heat(T_(80))or light(T_(70))stresses than the counterpart based on the NFA with dichlorinated terminal.Such advantages were inherited by the S-5Cl-based ternary device.Moreover,S-5Cl enabled a good efficiency of 17.66%with a remarkable fill factor of 81.69%for binary OPV and a much better efficiency of 19.25%for the ternary device.Therefore,our work indicates that tailoring the terminal groups for more condensed molecular arrangements of NFAs is a feasible route to highly efficient and stable OPVs.展开更多
Active learning(AL)is a powerful method for accelerating novel materials discovery but faces huge challenges for extracting physical meaning.Herein,we novelly apply an interpretable AL strategy to efficiently optimize...Active learning(AL)is a powerful method for accelerating novel materials discovery but faces huge challenges for extracting physical meaning.Herein,we novelly apply an interpretable AL strategy to efficiently optimize the photothermal conversion efficiency(PCE)of carbon dots(CDs)in photothermal therapy(PTT).An equivalent value(SHapley Additive exPlanations equivalent value[SHAP-EV])is proposed which explicitly quantifies the linear contributions of experimental variables to the PCE,derived from the joint SHAP values.The SHAP-EV,with an R2 of 0.960 correlated to feature’s joint SHAP,is integrated into the AL utility functions to enhance evaluation efficiency during optimization.Using this approach,we successfully synthesized irondoped CDs(Fe-CDs)with PCE exceeding 78.7%after only 16 experimental trials over four iterations.This achievement significantly advances the previously low PCE values typically reported for CDs.Furthermore,Fe-CDs demonstrated multienzyme-like activities,which could respond to the tumormicroenvironment(TME).In vitro and in vivo experiments demonstrate that Fe-CDs could enhance ferroptosis through synergistic PTT and chemodynamic therapy(CDT),thereby achieving remarkable antitumor efficacy.Our interpretable AL strategy offers new insights for accelerating bio-functional materials development in antitumor treatments.展开更多
Understanding the molecular packing arrangement and aggregation behaviors of organic semiconductor materials is crucial in comprehending their unique properties,particularly in complex structures required for solution...Understanding the molecular packing arrangement and aggregation behaviors of organic semiconductor materials is crucial in comprehending their unique properties,particularly in complex structures required for solution processing in organic photovoltaics.However,there has been limited focus on studying the diverse self-assembly behaviors induced by varying molecular skeletons.To address this issue,we designed and synthesized i-9R4Cl,i-7R4Cl,and 7R4Cl with nine-and seven-membered ring backbones,respectively.The single crystal structures revealed a standard H-type aggregate in i-9R4Cl,which is rare fully face-to-face packing in nonfullerene acceptors.Conversely,i-7R4Cl exhibited a typical J-type aggregate,while 7R4Cl demonstrated a synergistic H/J-type aggregate as conventional Y-series acceptors.Moreover,it reveals a unique three-dimensional(3D)network packing structure dominated by H-aggregation in i-9R4Cl,a linear packing structure in i-7R4Cl,and an elliptical 3D network packing structure in 7R4Cl.The grazing incidence wide-angle X-ray scattering tests confirmed that the packing arrangement in crystal structures was preserved in the film state.Despite i-9R4Cl’s favorable properties in stacking,it achieved a lower power conversion efficiency(PCE)of 1.97%compared to the other two acceptors,which should be attributed to poor exciton separation and carrier recombination induced by the morphology of aggregation regulation.Surprisingly,the electron paramagnetic resonance indicates that i-9R4Cl possesses radical properties,and when introduced as the third component in the PBDB-TF:BTIC-C9-4Cl based devices,it led to an enhancement in PCE from 18.42%to 19.08%,making it one of the highest efficiencies based on the BTIC-C9-4Cl system.It underscores how even subtle changes in molecular structure can significantly impact material properties.Our work aims to control the aggregation states of molecules,transitioning from standard H-type to J-type and to synergistic H/J-type aggregates,subsequently investigating the corresponding relationship between aggregation states,material properties,and devices performance.This is critical for designing new acceptor materials to overcome the bottlenecks in efficiency.展开更多
Honeycomb metastructures are widely used in electromagnetic wave absorption applications due to their lightweight and high-strength properties.While geometric modifications can further enhance microwave absorption,the...Honeycomb metastructures are widely used in electromagnetic wave absorption applications due to their lightweight and high-strength properties.While geometric modifications can further enhance microwave absorption,the unclear relationships between structural parameters,electromagnetic response,and mechanical performance present challenges for optimizing these structures to achieve both absorption and mechanical performance.This study introduces an automated framework for the bi-objective optimization of hybrid geometry honeycomb metastructures(HGHMs),fabricated with a graphene conductive coating and photosensitive resin for the honeycomb substrate,designed to improve both microwave absorption and mechanical resistance.By integrating artificial intelligence(AI),parametric modeling,and finite element analysis,a robust system was developed to explore the design space.Two optimized HGHM configurations were identified:One prioritizes microwave absorption with a-10 dB bandwidth of 6.1–18.0 GHz,a-15 dB bandwidth of 6.9–16.3 GHz,and a compressive Young's modulus of E=123 MPa,while the other balances absorption performance(-10 dB bandwidth:5.7–18.0 GHz)and mechanical robustness with E=638 MPa.Experimental validation confirmed the simulation results,and sensitivity analysis revealed the relationship between structural design,absorption,and deformation resistance.Based on a highaccuracy neural network surrogate model for the prediction of reflection loss curves,differential evolution was employed to suggest geometric parameters that lead to desired reflection loss curves.These results underscore the transformative potential of AI-based optimization for the rapid,automated,and customized design of multifunctional metastructures.展开更多
基金supported in part by National Key R&D Program of China under Grant 2024YFB4708600National Natural Science Foundation of China under Grant 52305304+3 种基金Jilin Youth Growth Technology Project under Grant 20230508147RCthe Science and Technology Research Project of Jilin Provincial Education Department(No.JJKH20231193KJ)supported in part by the National Natural Science Foundation of China under Grant 52021003 and Grant 52205565in part by the Natural Science Foundation of Jilin Province under Grant 20210101053JC.
文摘Traditional linear vibration isolators struggle to combine high load-bearing capacity with low-frequency vibration isolation, whereas nonlinear metastructure isolators can effectively fulfill both functions. This paper draws inspiration from the Quasi-Zero Stiffness (QZS) characteristics resulting from the buckling deformation of beams, and proposes a gear-based QZS structure by arranging beams in a circular array. We investigated the static mechanical behavior under different structural parameters, loading angles, and gear combinations through experiments and simulations, and demonstrated the mechanical performances could be effectively programmed. Subsequent vibration isolation tests on the double gears prove superior vibration isolation performance at low frequency while maintaining high load-bearing capacities. Additionally, a key contribution of our work is the development of a mathematical model to characterize the buckling behavior of the unit beam within the gear structure, with its accuracy validated through finite element analysis and experimental results. The gear’s modulus, number of teeth, and pressure angle are selected according to standard series, allowing the gear can be seamlessly integrated into existing mechanical systems in critical fields such as aerospace, military, and etc.
基金support by the Key Research Project of Zhejiang Laboratory(N.O.2021PE0AC02)the National Natural Science Foundation of China(N.O.11674210)the Project of Hetao Shenzhen-Hong Kong Science and Technology Innovation Cooperation Zone(HZQB-KCZYB-2020083).
文摘Photodetectors with long detection distances and fast response are important media in constructing a non-contact human-machine interface for the Masterly Internet of Things(MIT).All-inorganic perovskites have excellent optoelectronic performance with high moisture and oxygen resistance,making them one of the promising candidates for high-performance photodetectors,but a simple,low-cost and reliable fabrication technology is urgently needed.Here,a dual-function laser etching method is developed to complete both the lyophilic split-ring structure and electrode patterning.This novel split-ring structure can capture the perovskite precursor droplet efficiently and achieve the uniform and compact deposition of CsPbBr3 films.Furthermore,our devices based on laterally conducting split-ring structured photodetectors possess outstanding performance,including the maximum responsivity of 1.44×105 mA W^(−1),a response time of 150μs in 1.5 kHz and one-unit area<4×10-2 mm2.Based on these split-ring photodetector arrays,we realized three-dimensional gesture detection with up to 100 mm distance detection and up to 600 mm s^(−1) speed detection,for low-cost,integrative,and non-contact human-machine interfaces.Finally,we applied this MIT to wearable and flexible digital gesture recognition watch panel,safe and comfortable central controller integrated on the car screen,and remote control of the robot,demonstrating the broad potential applications.
基金R.Ma thanks the support from PolyU Distinguished Postdoc Fellowship(1-YW4C)Z.Luo thanks the National Natural Science Foundation of China(NSFC,No.22309119)+7 种基金J.Wu thanks the Guangdong government and the Guangzhou government for funding(2021QN02C110)the Guangzhou Municipal Science and Technology Project(No.2023A03J0097 and 2023A03J0003)H.Yan appreciates the support from the National Key Research and Development Program of China(No.2019YFA0705900)funded by MOST,the Basic and Applied Research Major Program of Guangdong Province(No.2019B030302007)the Shen Zhen Technology and Innovation Commission through(Shenzhen Fundamental Research Program,JCYJ20200109140801751)the Hong Kong Research Grants Council(research fellow scheme RFS2021-6S05,RIF project R6021-18,CRF project C6023‐19G,GRF project 16310019,16310020,16309221,and 16309822)Hong Kong Innovation and Technology Commission(ITC‐CNERC14SC01)Foshan‐HKUST(Project NO.FSUST19‐CAT0202)Zhongshan Municipal Bureau of Science and Technology(NO.ZSST20SC02)and Tencent Xplorer Prize。
文摘With plenty of popular and effective ternary organic solar cells(OSCs)construction strategies proposed and applied,its power conversion efficiencies(PCEs)have come to a new level of over 19%in single-junction devices.However,previous studies are heavily based in chloroform(CF)leaving behind substantial knowledge deficiencies in understanding the influence of solvent choice when introducing a third component.Herein,we present a case where a newly designed asymmetric small molecular acceptor using fluoro-methoxylated end-group modification strategy,named BTP-BO-3FO with enlarged bandgap,brings different morphological evolution and performance improvement effect on host system PM6:BTP-eC9,processed by CF and ortho-xylene(o-XY).With detailed analyses supported by a series of experiments,the best PCE of 19.24%for green solvent-processed OSCs is found to be a fruit of finely tuned crystalline ordering and general aggregation motif,which furthermore nourishes a favorable charge generation and recombination behavior.Likewise,over 19%PCE can be achieved by replacing spin-coating with blade coating for active layer deposition.This work focuses on understanding the commonly met yet frequently ignored issues when building ternary blends to demonstrate cutting-edge device performance,hence,will be instructive to other ternary OSC works in the future.
基金financial support the Key Research Project of Zhejiang Laboratory(2021PE0AC02)the National Natural Science Foundation of China(11704239,61922053,and 11674210)。
基金the support from the NSFC (22209131, 22005121, 21875182, and 52173023)National Key Research and Development Program of China (2022YFE0132400)+4 种基金Key Scientific and Technological Innovation Team Project of Shaanxi Province (2020TD-002)111 project 2.0 (BP0618008)Open Fund of Jiangsu Engineering Laboratory of Light-Electricity-Heat Energy-Converting Materials and Applications (Changzhou University, GDRGCS2022002)Open Fund of Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education (Jiangxi Normal University, KFSEMC-202201)acquired at beamlines 7.3.3 and 11.0.1.2 at the Advanced Light Source, which is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC0205CH11231
文摘Power-conversion-efficiencies(PCEs)of organic solar cells(OSCs)in laboratory,normally processed by spin-coating technology with toxic halogenated solvents,have reached over 19%.However,there is usually a marked PCE drop when the bladecoating and/or green-solvents toward large-scale printing are used instead,which hampers the practical development of OSCs.Here,a new series of N-alkyl-tailored small molecule acceptors named YR-SeNF with a same molecular main backbone are developed by combining selenium-fused central-core and naphthalene-fused endgroup.Thanks to the N-alkyl engineering,NIR-absorbing YR-SeNF series show different crystallinity,packing patterns,and miscibility with polymeric donor.The studies exhibit that the molecular packing,crystallinity,and vertical distribution of active layer morphologies are well optimized by introducing newly designed vip acceptor associated with tailored N-alkyl chains,providing the improved charge transfer dynamics and stability for the PM6:L8-BO:YRSeNF-based OSCs.As a result,a record-high PCE approaching 19%is achieved in the blade-coating OSCs fabricated from a greensolvent o-xylene with high-boiling point.Notably,ternary OSCs offer robust operating stability under maximum-power-point tracking and well-keep>80%of the initial PCEs for even over 400 h.Our alkyl-tailored vip acceptor strategy provides a unique approach to develop green-solvent and blade-coating processed high-efficiency and operating stable OSCs,which paves a way for industrial development.
基金financial support from the Guangzhou Municipal Government.
文摘Lithium metal batteries(LMBs)are considered the ideal choice for high volumetric energy density lithium-ion batteries,but uncontrolled lithium deposition poses a significant challenge to the stability of such devices.In this paper,we introduce a 2.5μm-thick asymmetric and ultrastrong separator,which can induce tissue-like lithium deposits.The asymmetric separator,denoted by utPE@Cu_(2)O,was prepared by selective synthesis of Cu_(2)O nanoparticles on one of the outer surfaces of a nanofibrous(diameter~10 nm)ultrastrong ultrahigh molecular weight polyethylene(UHMWPE)membrane.Microscopic analysis shows that the lithium deposits have tissue-like morphology,resulting in the symmetric lithium cells assembled using utPE@Cu_(2)O with symmetric Cu_(2)O coating exhibiting stable performance for over 2000 h of cycling.This work demonstrates the feasibility of a facile approach ultrathin separators for the deployment of lithium metal batteries,providing a pathway towards enhanced battery performance and safety.
基金supported by the Research Grants Council(26206115,16304821 and 16309418)the Southern Marine Science and Engineering Guangdong Laboratory(Guangzhou)(SMSEGL20SC01)+2 种基金the Innovation and Technology Commission(grant no.ITC-CNERC14EG03)of the Hong Kong Special Administrative Regionthe Hong Kong Postdoctoral Fellowship Scheme(HKUST PDFS2021-4S12 and HKUST PDFS2021-6S08)the support from the Shenzhen fundamental research funding(JCYJ20210324115809026,20200925154115001,JCYJ20200109141216566)。
文摘Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of urea.Herein,we report copper carbonate hydroxide(Cu_2(OH)_2CO_(3))as an efficient CO_(2)NO_(3)RR electrocatalyst with an impressive urea Faradaic efficiency of45.2%±2.1%and a high yield rate of 1564.5±145.2μg h~(-1)mg_(cat)~(-1).More importantly,H_(2) evolution is fully inhibited on this electrocatalyst over a wide potential range between-0.3 and-0.8 V versus reversible hydrogen electrode.Our thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu_2(OH)_2CO_(3) by combining the two intermediates,~*COOH and~*NHO.This work demonstrates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO_(2)NO_(3)RR,and provide guidance for rational design of more advanced catalysts.
基金supported by the National Natural Science Foundation of China (Grant Nos. 11991060, 12088101, 52172136, 12104035, and U2230402)。
文摘Transmutation is an efficient approach for material design. For example, ternary compound CuGaSe_(2) in chalcopyrite structure is a promising material for novel optoelectronic and thermoelectric device applications. It can be considered as formed from the binary host compound ZnSe in zinc-blende structure by cation transmutation(i.e., replacing two Zn atoms by one Cu and one Ga). While cation-transmutated materials are common, aniontransmutated ternary materials are rare, for example, Zn_(2)As Br(i.e., replacing two Se atoms by one As and one Br)is not reported. The physical origin for this puzzling disparity is unclear. In this work, we employ first-principles calculations to address this issue, and find that the distinct differences in stability between cation-transmutated(mix-cation) and anion-transmutated(mix-anion) compounds originate from their different trends of ionic radii as functions of their ionic state, i.e., for cations, the radius decreases with the increasing ionic state, whereas for anions, the radius increases with the increasing absolute ionic state. Therefore, for mix-cation compounds,the strain energy and Coulomb energy can be simultaneously optimized to make these materials stable. In contrast, for mix-anion systems, minimization of Coulomb energy will increase the strain energy, thus the system becomes unstable or less stable. Thus, the trend of decreasing strain energy and Coulomb energy is consistent in mix-cation compounds, while it is opposite in mix-anion compounds. Furthermore, the study suggests that the stability strategy for mix-anion compounds can be controlled by the ratio of ionic radii r3/r1, with a smaller ratio indicating greater stability. Our work, thus, elucidates the intrinsic stability trend of transmutated materials and provides guidelines for the design of novel ternary materials for various device applications.
基金financially supported by the Sichuan Science and Technology Program (2023YFH0086, 2023YFH0085, 2023YFH0087 and 2023NSFSC0990)the State Key Laboratory of Polymer Materials Engineering (sklpme2022-3-02 and sklpme2023-2-11)the Tibet Foreign Experts Program (2022wz002)
文摘Semitransparent organic photovoltaics(STOPVs)have gained wide attention owing to their promising applications in building-integrated photovoltaics,agrivoltaics,and floating photovoltaics.Organic semiconductors with high charge carrier mobility usually have planar and conjugated structures,thereby showing strong absorption in visible region.In this work,a new concept of incorporating transparent inorganic semiconductors is proposed for high-performance STOPVs.Copper(I)thiocyanate(CuSCN)is a visible-transparent inorganic semiconductor with an ionization potential of 5.45 eV and high hole mobility.The transparency of CuSCN benefits high average visible transmittance(AVT)of STOPVs.The energy levels of CuSCN as donor match those of near-infrared small molecule acceptor BTP-eC9,and the formed heterojunction exhibits an ability of exciton dissociation.High mobility of CuSCN contributes to a more favorable charge transport channel and suppresses charge recombination.The control STOPVs based on PM6/BTP-eC9 exhibit an AVT of 19.0%with a power conversion efficiency(PCE)of 12.7%.Partial replacement of PM6 with CuSCN leads to a 63%increase in transmittance,resulting in a higher AVT of 30.9%and a comparable PCE of 10.8%.
基金the National Natural Science Foundation of China(No.22122704 and No.22177067)the Program for Distinguished Professor of Shanghai Universities(Oriental Scholars),Tracking Plan GZ202209+1 种基金Shanghai Sailing Program(24YF2712500)and Guangzhou-HKUST(GZ)Joint Funding Program(No.2023A03J0003).
文摘G-quartet(G4)-based circularly polarized luminescence(CPL)materials within CPL engineering have attracted substantial attention in optoelectronics and photonics owing to their excellent chiral properties and promising applications in advanced optical devices.However,their practical use is limited by relatively low quantum yield(QY),which reduces emission efficiency.Addressing this challenge,we present BgoFace,an integrated active learning(AL)-based software,to optimize G4-based CPL materials with high QY.Starting with an initial dataset of 54 experimentally validated samples,the system executed six AL cycles encompassing 24 targeted experimental groups.Through this closed-loop workflow,BgoFace successfully identified G4 complexes exhibiting a near doubling of QY(37.25%).This achievement significantly advances the previously low QY values typically reported for G4-based CPL materials.The optimized materials demonstrate enhanced stability and processability,attributable to the AL algorithm's simultaneous consideration of multiple physicochemical parameters.This study not only advances the field of G4-based CPL materials for optical and photonic applications,but also establishes a generalizable AL framework suitable for optimizing functional nanomaterials in optoelectronic device design.By bridging datadriven design and experimental validation,BgoFace offers a transformative strategy for accelerating the development of functional nanomaterial engineering.
基金supported by the National Natural Science Foundation of China(22275058,U20A6002,21903017)the Ministry of Science and Technology of China(2019YFA0705900)+4 种基金the Guangdong Basic and Applied Basic Research Foundation(2022B15151-20008,2023A0505010003,2023A1515011500)the Guangdong Innovative and Entrepreneurial Research Team Program(2019ZT08L075)the Ningbo Natural Science Foundation(2024J111)the Scientific Research Fund of Zhejiang Provincial Education Department(Y202456587)the On Campus Research Projects at Guangzhou University(ZH2023005)。
文摘Fully non-fused electron acceptors(FNEAs)exhibit great potential as cost-effective electron acceptors for organic solar cells(OSCs).However,the device performance of FNEAs in OSCs is hindered by weak acceptor crystallinity associated with the rotation of carbon-carbon single bonds.Herein,we report the formation of strong molecular crystallinity of FNEAs and thus favorable fibril network morphology in blend films by finely optimizing the thermal annealing temperature.This favorable morphology not only enhanced the diffusion distance and dissociation efficiency of excitons in the acceptor phase,but also significantly boosted the electron mobility and carrier extraction rate.Consequently,a power conversion efficiency of 17.3%along with a short-circuit current density of 27.7 mA cm^(-2)are obtained,which are both the highest values for OSCs employing fully non-fused electron acceptors.These results demonstrate promising prospects and provide valuable insights for achieving high-efficiency OSCs using low-cost FNEAs.
基金the support from the Poly U Distinguished Postdoc Fellowship(1-YW4C)the Guangdong Basic and Applied Basic Research Foundation(2025A1515012147)+8 种基金the National Natural Science Foundation of China(12404480,12274303)the Shenzhen Science and Technology Program(JCYJ20240813113238050,JCYJ20240813113306008)the Shenzhen Key Laboratory of Applied Technologies of Super-Diamond and Functional Crystals(ZDSYS20230626091303007)for the supportthe Guangdong S&T Program(2022B1212040001)the Guangdong-Hong Kong-Macao Joint Laboratory(2023B1212120003)for the supportthe Guangdong Government and the Guangzhou Government(2021QN02C110)the Guangzhou Municipal Science and Technology Project(2023A03J0097,2023A03J0003)the National Natural Science Foundation of China(NSFC)(52303249)for the supportfunding by the Federal Institute for Research on Building,Urban Affairs and Spatial Development on behalf of the Federal Ministry of the Interior,Building and Community with funds from the Zukunft Bau Research Program under grant“Nachhaltige Sonnenschutzsysteme aus hochfester Zellulose zur Umwandlung von Sonnenenergie”。
文摘The development of power conversion efficiency(PCE)for organic solar cells(OSCs)based on polymer donors with benzo[1,2-b:4,5-b′]-difuran building block is slower than that of those based on benzodithiophene due to uncontrollable aggregation behavior.However,the former is expected to be more promising in realizing environmentally friendly and high-performance devices.Thereby,a smart aggregation tuning strategy is needed for boosting the efficiency of this type of OSCs.Here we report solid additives designed by self-imitation strategy,which aims to control the aggregation of the donor D18-Fu,and regulate the domain expansion of the acceptor L8-BO.Three oligomeric additives,with or without halogenation,can uniformly reduce the energy loss and enhance charge generation compared to an additive-free control device.This improvement is demonstrated through a series of morphological characterizations,photophysical analyses and theoretical simulations,indicating strong interaction between additive molecules and donor&acceptor.As a result,a 19%PCE is reported in binary OSCs,which also represents the highest level for devices based on benzo[1,2-b:4,5-b′]-difuran core contained polymer donor.Apart from high performance,our study provides new insights into manipulating the competition between the donor and acceptor's pure phase formation through new additive design methods.
基金the financial support from the National Natural Science Foundation of China(21805097)the Guangdong Natural Science Foundation(2021B1515120073)+6 种基金the Guangdong Provincial Science and Technology Foundation(2022A0505050068)Research Grants Council of Hong Kong(C4005-22YRGC Senior Research Fellowship Scheme(SRFS2223-5S01))the support from the Poly U Distinguished Postdoctoral Fellowship(1-YW4C)the funding support from the National Natural Science Foundation of China(52303249)the Department of Science and Technology of Guangdong Province(2021QN02C110)the Guangzhou Municipal Science and Technology Bureau Projects(2023A03J0097,2023A03J0003,2024A04J4513)。
文摘In this paper,an alkyl-chain-linked strategy is employed to synthesize a dimeric acceptor,DPhC8Y,which achieves simultaneous enhancements in device efficiency and stability while also exhibiting an unprecedentedly high production yield compared to other“giant molecular acceptors”for organic solar cells(OSCs).Compared to the monomer DTY6,DPhC8Y contains improved crystalline ordering and refined phase separation,thereby reducing non-radiative loss,suppressing bulk and interface recombination,and decreasing trap density.On the other hand,the dimer acceptor possesses an intrinsically higher glass transition point.Through performance evaluation,the binary device of D18:DPhC8Y blend demonstrates 19.50%efficiency with remarkably over 80%fill factor(FF),surpassing those of D18:DTY6(18.25%and 76.42%).Meanwhile,the dimer-based active layer displays significantly enhanced storage and thermal stability in the device.Our report showcases the possibility of achieving OSCs with concurrent decent efficiency,stability,and cost-effectiveness through smart material and synthesis design.
基金supported by the National Key Research and Development Program of China(Grant No.2022YFB3707803)the National Natural Science Foundation of China(Grants Nos.12072179 and 11672168)+2 种基金the Key Research Project of Zhejiang Lab(Grant No.2021PE0AC02)Shanghai Pujiang Program(Grant No.23PJ1403500)Shanghai Engineering Research Center for Integrated Circuits and Advanced Display Materials.
文摘Accelerating the discovery of advanced materials is crucial for modern industries,aerospace,biomedicine,and energy.Nevertheless,only a small fraction of materials are currently under experimental investigation within the vast chemical space.Materials scientists are plagued by timeconsuming and labor-intensive experiments due to lacking efficient material discovery strategies.Artificial intelligence(AI)has emerged as a promising instrument to bridge this gap.Although numerous AI toolkits or platforms for material science have been developed,they suffer from many shortcomings.These include primarily focusing on material property prediction and being unfriendly to material scientists lacking programming experience,especially performing poorly with limited data.Here,we developed MLMD,an AI platformfor materials design.It is capable of effectively discovering novel materials with high-potential advanced properties end-to-end,utilizing model inference,surrogate optimization,and even working in situations of data scarcity based on active learning.Additionally,it integrates data analysis,descriptor refactoring,hyper-parameters auto-optimizing,and properties prediction.It also provides a web-based friendly interface without need programming and can be used anywhere,anytime.MLMD is dedicated to the integration of material experiment/computation and design,and accelerate the new material discovery with desired one or multiple properties.It demonstrates the strong power to direct experiments on various materials(perovskites,steel,high-entropy alloy,etc).MLMD will be an essential tool for materials scientists and facilitate the advancement of materials informatics.
基金supported by the project Mechanical Engineering of Biological and Bio-inspired Systems(No.CZ.02.01.01/00/22_008/0004634)by Programme Johannes Amos Comenius,call Excellent Research.
文摘The present study introduces a tribological comparison of five polyvinyl alcohol(PVA)hydrogel specimens with different physiological properties and possible candidate materials for cartilage replacement.The superior lubrication of articular cartilage is believed to lie in solid-to-solid molecular interactions.Therefore,the focus was paid to the investigation of boundary lubrication with regard to interstitial fluid flow reduction.The experiments were carried out in a ball-on-plate(glass-on-hydrogel)configuration.Based on the experiments,we proposed a boundary lubrication mechanism,selected a hydrogel with the least surface damage,and highlighted the desired properties that should be considered when developing the artificial cartilage.
基金sponsored by the Shanghai Pujiang Program(Grant no.20PJ1403700)the Guangzhou-HKUST(GZ)Joint Funding Program(nos.2023A03J0003 and 2023A03J0103)the Opening Project Fund of Materials Service Safety Assessment Facilities(MSAF-2024-107).
文摘We present a multi-objective Bayesian active learning strategy,which greatly accelerates the discovery of super high-strength and high-ductility lead-free solder alloys.The active learning strategy demonstrates that a machine learning model will have high generalizability if experimental data uncertainty is included,which greatly improves the model prediction or the material design accuracy.The feature-point-start forward method in multi-objective optimization adopts two Gaussian process regression(GPR)models,one for strength and one for elongation,and their outputs build up the acquisition-function-modified objective space of strength and elongation.Then,Bayesian sampling is applied to design the next experiments by balancing exploitation and exploration.Seven multi-objective active learning iterations discovered two novel super high-strength and high-ductility lead-free solder alloys.After that,various material characterizations were conducted on the two novel solder alloys,and the results exhibited their high performances in melting properties,wettability,electrical conductivity,and shear strength of the solder joint and explored the mechanism of high strength and high ductility of the alloys.The present work systematically analyzes the important role of experimental uncertainty in machine learning,especially in the global optimization for material design,which demands high generalizability of predictions.
基金supported by the National Natural Science Foundation of China(grant nos.22279114,52473197,52273199,52321165650,and 52394274)the Fundamental Research Funds for the Central Universities(grant nos.226-2024-00005 and 226-2024-00056).
文摘The A-D-A and A-D-A'-D-A molecular skeletons of nonfullerene acceptors(NFAs)establish the success in realizing high-efficiency organic photovoltaics(OPVs),while the C=C bond between D and A moieties stands as a critical weakness for long-term stability.Herein,we report that by developing trichlorinated cyanoindone as A terminal,the resulting NFA denoted S-5Cl could resist both photodegradation with an increased rotational energy barrier and thermo-diffusion with the elevated glass transition temperature,which was further supported by tighter molecular stacking in the single crystal of S-5Cl.These features,thus,allow the S-5Cl-based binary OPV to possess 2–4 times longer lifetimes under heat(T_(80))or light(T_(70))stresses than the counterpart based on the NFA with dichlorinated terminal.Such advantages were inherited by the S-5Cl-based ternary device.Moreover,S-5Cl enabled a good efficiency of 17.66%with a remarkable fill factor of 81.69%for binary OPV and a much better efficiency of 19.25%for the ternary device.Therefore,our work indicates that tailoring the terminal groups for more condensed molecular arrangements of NFAs is a feasible route to highly efficient and stable OPVs.
基金funded by the National Natural Science Foundation of China(22122704 and 22177067)the Program for Distinguished Professor of Shanghai Universities(Oriental Scholars),Tracking Plan GZ202209the Guangzhou-HKUST(GZ)Joint Funding Program(2023A03J0003).
文摘Active learning(AL)is a powerful method for accelerating novel materials discovery but faces huge challenges for extracting physical meaning.Herein,we novelly apply an interpretable AL strategy to efficiently optimize the photothermal conversion efficiency(PCE)of carbon dots(CDs)in photothermal therapy(PTT).An equivalent value(SHapley Additive exPlanations equivalent value[SHAP-EV])is proposed which explicitly quantifies the linear contributions of experimental variables to the PCE,derived from the joint SHAP values.The SHAP-EV,with an R2 of 0.960 correlated to feature’s joint SHAP,is integrated into the AL utility functions to enhance evaluation efficiency during optimization.Using this approach,we successfully synthesized irondoped CDs(Fe-CDs)with PCE exceeding 78.7%after only 16 experimental trials over four iterations.This achievement significantly advances the previously low PCE values typically reported for CDs.Furthermore,Fe-CDs demonstrated multienzyme-like activities,which could respond to the tumormicroenvironment(TME).In vitro and in vivo experiments demonstrate that Fe-CDs could enhance ferroptosis through synergistic PTT and chemodynamic therapy(CDT),thereby achieving remarkable antitumor efficacy.Our interpretable AL strategy offers new insights for accelerating bio-functional materials development in antitumor treatments.
基金supported by the National Natural Science Foundation of China(grant nos.22225504,22305112,and 22305114)Guangdong Provincial Key Laboratory of Catalysis(grant no.2020B121201002)+2 种基金Shenzhen Fundamental Research Program(grant no.JCYJ20210324120010028)China Postdoctoral Science Foundation(grant no.2022M721466)High level of special funds(grant no.G03050K002).
文摘Understanding the molecular packing arrangement and aggregation behaviors of organic semiconductor materials is crucial in comprehending their unique properties,particularly in complex structures required for solution processing in organic photovoltaics.However,there has been limited focus on studying the diverse self-assembly behaviors induced by varying molecular skeletons.To address this issue,we designed and synthesized i-9R4Cl,i-7R4Cl,and 7R4Cl with nine-and seven-membered ring backbones,respectively.The single crystal structures revealed a standard H-type aggregate in i-9R4Cl,which is rare fully face-to-face packing in nonfullerene acceptors.Conversely,i-7R4Cl exhibited a typical J-type aggregate,while 7R4Cl demonstrated a synergistic H/J-type aggregate as conventional Y-series acceptors.Moreover,it reveals a unique three-dimensional(3D)network packing structure dominated by H-aggregation in i-9R4Cl,a linear packing structure in i-7R4Cl,and an elliptical 3D network packing structure in 7R4Cl.The grazing incidence wide-angle X-ray scattering tests confirmed that the packing arrangement in crystal structures was preserved in the film state.Despite i-9R4Cl’s favorable properties in stacking,it achieved a lower power conversion efficiency(PCE)of 1.97%compared to the other two acceptors,which should be attributed to poor exciton separation and carrier recombination induced by the morphology of aggregation regulation.Surprisingly,the electron paramagnetic resonance indicates that i-9R4Cl possesses radical properties,and when introduced as the third component in the PBDB-TF:BTIC-C9-4Cl based devices,it led to an enhancement in PCE from 18.42%to 19.08%,making it one of the highest efficiencies based on the BTIC-C9-4Cl system.It underscores how even subtle changes in molecular structure can significantly impact material properties.Our work aims to control the aggregation states of molecules,transitioning from standard H-type to J-type and to synergistic H/J-type aggregates,subsequently investigating the corresponding relationship between aggregation states,material properties,and devices performance.This is critical for designing new acceptor materials to overcome the bottlenecks in efficiency.
基金supported by the National Key Research and Development Program of China(Grant No.2022YFB3707800)the“Artificial Intelligence Empowering Scientific Research Plan”initiative of the Shanghai Municipal Education Commissionthe National Natural Science Foundation of China(Grant Nos.12072179,12421002,52231007,12327804)。
文摘Honeycomb metastructures are widely used in electromagnetic wave absorption applications due to their lightweight and high-strength properties.While geometric modifications can further enhance microwave absorption,the unclear relationships between structural parameters,electromagnetic response,and mechanical performance present challenges for optimizing these structures to achieve both absorption and mechanical performance.This study introduces an automated framework for the bi-objective optimization of hybrid geometry honeycomb metastructures(HGHMs),fabricated with a graphene conductive coating and photosensitive resin for the honeycomb substrate,designed to improve both microwave absorption and mechanical resistance.By integrating artificial intelligence(AI),parametric modeling,and finite element analysis,a robust system was developed to explore the design space.Two optimized HGHM configurations were identified:One prioritizes microwave absorption with a-10 dB bandwidth of 6.1–18.0 GHz,a-15 dB bandwidth of 6.9–16.3 GHz,and a compressive Young's modulus of E=123 MPa,while the other balances absorption performance(-10 dB bandwidth:5.7–18.0 GHz)and mechanical robustness with E=638 MPa.Experimental validation confirmed the simulation results,and sensitivity analysis revealed the relationship between structural design,absorption,and deformation resistance.Based on a highaccuracy neural network surrogate model for the prediction of reflection loss curves,differential evolution was employed to suggest geometric parameters that lead to desired reflection loss curves.These results underscore the transformative potential of AI-based optimization for the rapid,automated,and customized design of multifunctional metastructures.
