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Highly efficient solution-processed organic photovoltaics enabled by improving packing behavior of organic semiconductors

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science China Chemistry 2024年第3期67卷 890-897页

作者： Xinyue Cui Hongxiang Li Hao Lu Yuqiang Liu Guangliu Ran Rui Liu Huarui Zhang Xueqing Ma Dawei Li Yi Lin Jifa Yu Wenkai Zhang Lei Cai Yahui Liu Pei Cheng Andong Zhang Zaifei Ma Guanghao Lu Zhishan Bo College of Textiles and Clothing State Key Laboratory of Bio-fibers and Eco-textilesQingdao UniversityQingdao 266071China State Key Laboratory of Polymer Materials Engineering College of Polymer Science and EngineeringSichuan UniversityChengdu 610065China Department of Physics and Applied Optics Beijing Area Major Laboratory Center for Advanced Quantum StudiesBeijing Normal UniversityBeijing 100875China Shandong Province Key Laboratory of Medical Physics and Image Processing Technology School of Physics and ElectronicsShandong Normal UniversityJinan 250014China Beijing Key Laboratory of Energy Conversion and Storage Materials College of ChemistryBeijing Normal UniversityBeijing 100875China Center for Advanced Low-Dimension Materials State Key Laboratory for Modification of Chemical Fibers and Polymer MaterialsCollege of Materials Science and EngineeringDonghua UniversityShanghai 201620China Frontier Institute of Science and Technology Xi'an Jiaotong UniversityXi'an 710054China

Solution processability is a unique property of organic semiconductors. The compact and regular π-π stacking between molecules is paramount in the performance of organic optoelectronic devices. However, it is still a challenge to improve their stacking quality without sacrificing the solution-processability from the aspect of materials design. Here, delicately engineered additives are presented to promote the formation of ordered aggregation of conjugated molecules by regulating their nucleation and growth dynamics. Intriguingly, the long-chain BTP-eC9-4F molecules can realize ordered aggregation comparable to short-chain ones without sacrificing processability. The domain size of BTP-eC9-4F aggregation is enlarged from 24.2 to 32.2 nm in blend *** exciton diffusion and charge transport become faster, contributing to the suppression of recombination losses. As a result, a power conversion efficiency of 19.2% is achieved in D18:BTP-eC9-4F based organic photovoltaics. Our findings demonstrate a facile strategy to improve the packing quality of solution-processed organic semiconductors for high-efficiency photovoltaics and beyond photovoltaics.

关键词： organic semiconductor organic photovoltaic charge transport solution processability

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Multifunction integration within magnetic CNT-bridged MXene/CoNi based phase change materials

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escience 2024年第6期4卷 108-117页

作者： Yan Gao Xiao Chen Xu Jin Chenjun Zhang Xi Zhang Xiaodan Liu Yinhui Li Yang Li Jinjie Lin Hongyi Gao Ge Wang Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory of Function Materials for Molecule&Structure ConstructionSchool of Materials Science and EngineeringUniversity of Science and Technology BeijingBeijing 100083China School of Physics and Astronomy Beijing Normal UniversityBeijing 100875China Research Institute of Petroleum Exploration&Development PetroChinaBeijing 100083China Micro-Nano System Research Center College of Information and Optical EngineeringTaiyuan University of TechnologyTaiyuanShanxi 030024China Shunde Graduate School University of Science and Technology BeijingShunde 528399China

Developing advanced nanocomposite phase change materials(PCMs)integrating zero-energy thermal management,microwave absorption,photothermal therapy and electrical signal detection can promote the leapfrog development of flexible wearable electronic *** this goal,we propose a multidimensional collaborative strategy combining two-dimensional(2D)MXene nanosheets with metal-organic framework-derived onedimensional(1D)carbon nanotubes(CNTs)and zero-dimensional(0D)metal *** encapsulating paraffin wax(PW)in three-dimensional(3D)networked multidimensional MXene/CoNi-C,the resulting composite PCMs exhibit excellent thermal energy storage capacity and long-term thermally reliable *** from the synergistically enhanced photothermal effects of CNTs,Co/Ni nanoparticles and MXene,PW@MXene/CoNi-C can capture photons efficiently and transfer phonons quickly,yielding an ultrahigh photothermal conversion and storage efficiency of 97.5%.Additionally,PW@MXene/CoNi-C composite PCMs exhibit high microwave absorption with a minimum reflection loss of -49.3 dB at 8.03 GHz in heat-related electronic application *** attractively,the corresponding flexible phase change film can simultaneously achieve thermal management and electromagnetic shielding of electronic devices,as well as photothermal therapy and electrical signal detection for *** functional integration design provides an important reference for developing advanced flexible multifunctional wearable materials and devices.

关键词： Phase change materials Metal-organic frameworks Two-dimensional MXene Photothermal conversion Thermal energy storage Microwave absorption

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Spin-dependent terahertz wavefront shaping based on hybrid phase in all-silicon chiral metasurfaces

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光子学研究（英文） 2025年第5期13卷 1271-1281页

作者： JIE LI LELING CHEN HANG XU TONG NAN XUEGUANG LU HUI LI WENHUI XU QI TAN JITAO LI YUANYUAN LV TINGTING LIU SHUYUAN XIAO TINGTING TANG LI LUO WANXIA HUANG JIN HE YAN ZHANG JIANQUAN YAO Sichuan Meteorological Optoelectronic Sensor Technology and Application Engineering Research Center College of Optoelectronic EngineeringChengdu University of Information TechnologyChengdu 610225China School of Precision Instruments and Opto-Electronics Engineering Tianjin UniversityTianjin 300072China Key Laboratory of Terahertz Optoelectronics Ministry of EducationDepartment of PhysicsCapital Normal UniversityBeijing 100048China College of Materials Science and Engineering Sichuan UniversityChengdu 610065China Sichuan Meteorological Optoelectronic Sensor Technology and Application Engineering Research Center College of Optoelectronic EngineeringChengdu University of Information TechnologyChengdu 610225China School of Precision Instruments and Opto-Electronics Engineering Tianjin UniversityTianjin 300072China School of Information Engineering Nanchang UniversityNanchang 330031China

Independent manipulation of orthogonal circularly polarized wavefronts is one of the important goals for meta-optics,and chiral nanophotonics is one of the crucial *** this article,we propose a new scheme for spin-dependent terahertz wavefront shaping based on chiral metasurfaces,which involves a hybrid design of the propagation phase,chirality induced phase,and Pancharatnam-Berry phase in all-silicon meta-atoms.A control-lable linear polarization conversion effect in the transmitted wave is obtained via breaking the mirror symmetry and preserving the C2 symmetry of the resonator,which causes a different form of the Jones *** simulta-neously adjusting the in-plane geometric dimensions and azimuth angle of chiral units,and utilizing the evolution characteristics of circularly polarized components in parameter space and polarization space,spin-dependent phase responses have been *** provide the main theoretical analysis and demonstrate the functional design of circularly polarized multiplexed beam deflection or vortex beam generation,through the expected sim-ulation and experimental results near the operating frequency of 0.6 *** results may enrich the design of terahertz polarization-multiplexed devices.

关键词： terahertz hybrid phase all-silicon based chiral metasurfaces shaping spin-dependent wavefront

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Enhanced reversibility of the magnetoelastic transition in(Mn,Fe)2(P,Si)alloys via minimizing the transition-induced elastic strain energy

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Journal of Materials science & technology 2022年第8期103卷 165-176页

作者： Xuefei Miao Yong Gong Fengqi Zhang Yurong You Luana Caron Fengjiao Qian Wenhui Guo Yujing Zhang Yuanyuan Gong Feng Xu Niels van Dijk Ekkes Brück MIIT Key Laboratory of Advanced Metallic and Intermetallic Materials Technology School of Materials Science and EngineeringNanjing University of Science and TechnologyNanjing 210094China Fundamental Aspects of Materials and Energy Department of Radiation Science and TechnologyDelft University of TechnologyMekelweg 15DelftJB 2629Netherlands Department of Physics Bielefeld UniversityBielefeld 33501Germany Helmholtz-Zentrum Berlin für Materialien und Energie Berlin 12489Germany College of Physics Nanjing University of Aeronautics and AstronauticsNanjing 210016China

Magnetocaloric materials undergoing reversible phase transitions are highly desirable for magnetic refrigeration applications.(Mn,Fe)_(2)(P,Si)alloys exhibit a giant magnetocaloric effect accompanied by a magnetoelastic transition,while the noticeable irreversibility causes drastic degradation of the magnetocaloric properties during consecutive cooling *** the present work,we performed a comprehensive study on the magnetoelastic transition of the(Mn,Fe)_(2)(P,Si)alloys by high-resolution transmission electron microscopy,in situ field-and temperature-dependent neutron powder diffraction as well as density functional theory calculations(DFT).We found a generalized relationship between the thermal hysteresis and the transition-induced elastic strain energy for the(Mn,Fe)_(2)(P,Si)*** thermal hysteresis was greatly reduced from 11 to 1 K by a mere 4 at.%substitution of Fe by Mo in the Mn_(1.15)Fe_(0.80)P_(0.45)Si_(0.55)*** reduction is found to be due to a strong reduction in the transition-induced elastic strain *** significantly enhanced reversibility of the magnetoelastic transition leads to a remarkable improvement of the reversible magnetocaloric properties,compared to the parent *** on the DFT calculations and the neutron diffraction experiments,we also elucidated the underlying mechanism of the tunable transition temperature for the(Mn,Fe)_(2)(P,Si)family,which can essentially be attributed to the strong competition between the covalent bonding and the ferromagnetic exchange *** present work provides not only a new strategy to improve the reversibility of a first-order magnetic transition but also essential insight into the electron-spin-lattice coupling in giant magnetocaloric materials.

关键词： Magnetocaloric effect (Mn Fe)2(P Si) Hysteresis Neutron diffraction

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Thermodynamically induced crystal restructuring to make CsPbCl_(3) single crystal films for weak light detection

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Nano Research 2024年第11期17卷 9775-9783页

作者： Xiyan Pan Tai An Jie Sun Hua Dong Zhu Ma Guangxing Liang Yongbo Yuan Yang Li Wuqiang Wu Yong Ding Liming Ding Center for Excellence in Nanoscience (CAS) Key Laboratory of Nanosystem and Hierarchical Fabrication (CAS) National Center for Nanoscience and Technology Beijing 100190 China University of Chinese Academy of Sciences Beijing 100049 China School of Electronic Science and Engineering Xi’an Jiaotong University Xi’an 710049 China School of New Energy and Materials Southwest Petroleum University Chengdu 610500 China College of Physics and Optoelectronic Engineering Shenzhen University Shenzhen 518060 China School of Physics and Electronics Central South University Changsha 410083 China School of Energy and Power Jiangsu University of Science and Technology Zhenjiang 212000 China School of Chemistry Sun Yat-sen University Guangzhou 510006 China Beijing Key Laboratory of Novel Thin-Film Solar Cells North China Electric Power University Beijing 102206 China

CsPbCl_(3) perovskite is considered a highly promising material for ultraviolet (UV) photodetectors due to its exceptional thermal stability and excellent short-wavelength light response. However, its high lattice energy and low polarizability result in extremely low solubility in conventional solvents, making the synthesis of CsPbCl_(3) single crystals a significant challenge. In this study, we propose a novel thermodynamically induced crystal restructuring (TICR) process that can transform microcrystalline films (MCFs) into single crystal films (SCFs) within a short period. This method, for the first time, has successfully achieved the synthesis of centimeter-sized CsPbCl_(3) SCFs and the mechanism has been explored in depth using in-situ techniques. Furthermore, we report the first instance of a CsPbCl_(3) SCF UV photodiode, which exhibits a record-breaking on/off ratio of 3.32 × 10^(7) and a detectivity of up to 1.15 × 10^(14) Jones under 0 V bias. It demonstrates excellent response even under weak light conditions of 10 nW·cm^(−2) and maintains outstanding stability with almost no performance degradation after 15 months. This study provides a novel approach for the synthesis of perovskite single crystals and holds significant potential for advancing the development of high-performance optoelectronic devices.

关键词： CsPbCl3 single crystal film crystal restructuring photodiode ultraviolet detector

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Modulating perovskite crystallization and band alignment using coplanar molecules for high-performance indoor photovoltaics

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Journal of Energy Chemistry 2024年第11期98卷 383-390页

作者： Qu Yang Shuhan Fan Haozhe Zhang Zhenhuang Su Xingyu Gao Hui Shen Mingkui Wang Xiu Gong College of Physics &Guizhou Province Key Laboratory for Photoelectrics Technology and ApplicationGuizhou UniversityGuiyang 550025GuizhouChina State Key Laboratory of Public Big Data Guizhou UniversityGuiyang 550025GuizhouChina Shanghai Synchrotron Radiation Facility(SSRF) Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China Wuhan National Laboratory for Optoelectronics School of Optical and Electronic InformationHuazhong University of Science and TechnologyWuhan 430074HubeiChina

The proper bandgap and exceptional photostability enable CsPbI_(3) as a potential candidate for indoor photovoltaics(IPVs),but indoor power conversion efficiency(PCE) is impeded by serious nonradiative recombination stemming from challenges in incomplete DMAPbI_(3) conversion and lattice structure ***,the coplanar symmetric structu re of hexyl sulfide(HS) is employed to functionalize the CsPbI_(3) layer for fabricating highly efficient *** hydrogen bond between HS and DMAI promotes the conversion of DMAPbI_(3) to CsPbI_(3),while the copianar symmetric structure enhances crystalline ***,surface sulfidation during HS-induced growth results in the in situ formation of PbS,spontaneously creating a CsPbI_(3) N-P homojunction to enhance band alignment and carrier *** a result,the CsPbI_(3)&HS devices achieve an impressive indoor PCE of 39.90%(P_(in):334.6 μW cm^(-2),P_(out):133.5 μW cm^(-2)) under LED@2968 K,1062 lux,and maintain over 90% initial PCE for 800 h at ^(3)0% air ambient humidity.

关键词： Perovskite indoor photovoltaics CsPbI_(3) Coplanar symmetric structure molecules Crystallization kinetics Hydrogen bond N-P homojunction

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A general and facile calcination method to synthesize single-site catalysts for highly efficient electrochemical CO_(2) reduction

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Nano Research 2024年第5期17卷 3895-3901页

作者： Rui Sui Bingyan Wang Yongsheng Wang Jiajing Pei Wei Zhu Wenxing Chen Chunhui Li Ailing Sun Zhongbin Zhuang Engineering Research Center of Advanced Rare Earth Materials Department of ChemistryTsinghua UniversityBeijing 100084China College of Chemistry and Green Catalysis Center Zhengzhou UniversityZhengzhou 450001China State Key Lab of Organic-Inorganic Composites and Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical TechnologyBeijing 100029China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China Energy&Catalysis Center School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China

The electrochemical CO_(2) reduction reaction(CO_(2)RR)has received widespread attention as a promising method for producing sustainable chemicals and mitigating the global ***,we demonstrate a general and facile synthetic route for the metal-nitrogen-carbon(M-N-C)type catalyst by simply calcinating metal acetate and urea with commercial carbon black,which have potential application in CO_(2)*** synthesized Ni-NC-600 catalyst has the structure of single Ni atom coordinated with one N atom and three C atoms(Ni-N_(1)C_(3)),which is suggested by X-ray absorption *** Ni-NC-600 catalyst exhibits high CO_(2)RR catalytic performance and a high CO Faraday efficiency above 98%in a wide potential range from-0.7 to-1.3 V(*** hydrogen electrode(RHE)),superior to most of the reported Ni-N-C *** work has developed a facile strategy to synthesize high performance CO_(2)RR catalyst.

关键词： nickel single atom catalyst CO_(2)reduction reaction CO production electrocatalyst

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Chiral N-triflylphosphoramide-catalyzed asymmetric hydroamination of unactivated alkenes: a hetero-ene reaction mechanism

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Organic Chemistry Frontiers 2022年第6期9卷 1649-1661页

作者： Na Wang Li-Wen Fan Jin Zhang Qiang-Shuai Gu Jin-Shun Lin Guo-Qiang Chen Xin-Yuan Liu Peiyuan Yu College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518071China College of Physics and Optoelectronic Engineering Shenzhen UniversityShenzhen 518060China Department of Chemistry and Shenzhen Grubbs Institute Guangdong Provincial Key Laboratory of CatalysisSouthern University of Science and TechnologyShenzhen 518055China Academy for Advanced Interdisciplinary Studies and Department of Chemistry Southern University of Science and TechnologyShenzhen 518055China

A highly enantioselective intramolecular hydroamination reaction catalyzed by chiralN-triflylphosphoramide (NTPA) that features an exceptionally broad substrate scope of isolated unactivated alkenes was recently reported by some of us. Herein we report a detailed density functional theory(DFT) study that unveil an uncommon hetero-ene reaction mechanism for this transformation. The reaction changes from a stepwise mechanism involving discrete tertiary carbocation formation to a concertedmechanism to avoid the generation of energetically unfavorable secondary carbocation species for distinctly substituted alkene substrates. The reactivity of this reaction is primarily affected by the substituentson the internal carbon of the alkene, with the carbocation-stabilizing ones promoting the reaction. Inaddition, the reaction is also influenced by the substituents on the terminal alkene carbons: those diminishing the innate alkene polarization of the starting alkenes retard the reaction by disfavoring the formation of related transition states featuring highly polarized alkene residues. The steric effect of all thesealkene substituents was found to be largely unimportant due to the unique arrangement of the heteroene reaction complex that keeps the reacting alkene away from the sterically congested core region ofthe catalyst pocket. The lower acidity of chiral phosphoric acids than that of chiral NTPAs renders the protonated precomplex along the hetero-ene reaction pathway greatly thermodynamically disfavored. Thisindirectly results in a greater relative distortion in the corresponding transition state, which in turn causesreaction retardation. Our results demonstrate the use of intramolecular pericyclic reactions as an alternative strategy for alkene activation by chiral Brønsted acid catalysis and provide insights into the furtherdevelopment of asymmetric hydrofunctionalization of unactivated alkenes.

关键词： mechanism substituent asymmetric

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Practically Enhanced Hyperentanglement Concentration for Polarization-Spatial Hyperentangled Bell States with Linear Optics and Common Single-Photon Detectors

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Physical Review Applied 2023年第3期19卷 034044-034044页

作者： Gui-Long Jiang Wen-Qiang Liu Hai-Rui Wei School of Mathematics and Physics University of Science and Technology Beijing Beijing 100083 China Center for Quantum Technology Research and Key Laboratory of Advanced Optoelectronic Quantum Architecture and Measurements (MOE) School of Physics Beijing Institute of Technology Beijing 100081 China

Hyperentanglement, defined as the simultaneous entanglement in several independent degrees of freedom (DOFs) of a quantum system, is a fascinating resource in quantum information processing with its outstanding merits. Here we propose heralded hyperentanglement concentration protocols (hyper-ECPs) to concentrate an unknown partially less polarization-spatial hyperentangled Bell state with available linear optics and common single-photon detectors. By introducing time-delay DOFs, the schemes are highly efficient in that the success of the scheme can be accurately heralded by the detection signatures, and postselection techniques or photon-number-resolving detectors, necessary for previous experiments, are not required. Additionally, our linear optical architectures allow certain states, where concentration fails, to be recyclable, and a trick makes the success probabilities of our schemes higher than those of previous linear optical hyper-ECPs.

关键词： Entanglement manipulation Optical quantum information processing optoelectronics Photonics Polarization of light Quantum protocols Optical sources & detectors Single-photon detectors

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Quantum phase transition and critical behavior between the gapless topological phases

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Physical Review A 2024年第6期109卷 062226-062226页

作者： Hao-Long Zhang Han-Ze Li Sheng Yang Xue-Jia Yu Fujian Key Laboratory of Quantum Information and Quantum Optics College of Physics and Information Engineering Institute for Quantum Science and Technology Department of Physics School of Physics and Optoelectronics Institute for Advanced Study in Physics and School of Physics

The phase transition between gapped topological phases represents a class of unconventional criticality beyond the Landau paradigm. However, recent research has shifted attention to topological phases without a bulk gap, where the phase transitions between them are still elusive. In this work, based on large-scale density-matrix renormalization-group techniques, we investigate the critical behaviors of the extended quantum XXZ model obtained by the Kennedy-Tasaki transformation. Using fidelity susceptibility as a diagnostic, we obtain a complete phase diagram, which includes both topological nontrivial and trivial gapless phases. Furthermore, as the XXZ-type anisotropy parameter Δ varies, both the critical points hc and correlation length exponent ν remain the same as in the Δ=0 case, characterized by c=3/2 (Ising plus free boson) conformal field theory. Our results indicate that fidelity susceptibility can effectively detect and reveal a stable unconventional critical line between the topologically distinct gapless phases for general Δ. This work serves as a valuable reference for further research on phase transitions within the gapless topological phase of matter.

关键词： Continuous phase transition Quantum phase transitions Topological phases of matter Critical exponents Density matrix renormalization group

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