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Cooperation and Competition in Synchronous Open Quantum Systems

physical Review Letters 2023年第3期131卷 030401-030401页

作者： Taufiq Murtadho Sai Vinjanampathy Juzar Thingna Center for Theoretical Physics of Complex Systems Institute for Basic Science (IBS) Daejeon 34126 Republic of Korea Basic Science Program Korea University of Science and Technology Daejeon 34113 Republic of Korea School of Physical and Mathematical Sciences Nanyang Technological University 637371 Singapore Department of Physics Indian Institute of Technology-Bombay Powai Mumbai 400076 India Centre of Excellence in Quantum Information Computation Science and Technology Indian Institute of Technology Bombay Powai Mumbai 400076 India Centre for Quantum Technologies National University of Singapore 3 Science Drive 2 Singapore Singapore Department of Physics and Applied Physics University of Massachusetts Lowell Massachusetts 01854 USA

Synchronization between limit cycle oscillators can arise through entrainment to an external drive or through mutual coupling. The interplay between the two mechanisms has been studied in classical synchronizing systems, but not in quantum systems. Here, we point out that competition and cooperation between the two mechanisms can occur due to phase pulling and phase repulsion in quantum systems. We study their interplay in collectively driven degenerate quantum thermal machines and show that these mechanisms either cooperate or compete depending on the working mode of the machine (refrigerator or engine). The entrainment-mutual synchronization interplay persists with an increase in the number of degenerate levels, while in the thermodynamic limit of degeneracy, mutual synchronization dominates. Overall, our work investigates the effect of degeneracy and multilevel scaling of quantum synchronization and shows how different synchronizing mechanisms can cooperate and compete in quantum systems.

关键词： Masers Open quantum systems & decoherence Quantum statistical mechanics Synchronization Quantum heat engines & refrigerators

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Quantum-parametric-oscillator heat engines in squeezed thermal baths: Foundational theoretical issues

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physical Review E 2022年第1期105卷 014108-014108页

作者： Onat Arısoy Jen-Tsung Hsiang Bei-Lok Hu Chemical Physics Program and Institute for Physical Science and Technology University of Maryland College Park Maryland 20742 USA Center for High Energy and High Field Physics National Central University Taoyuan 320317 Taiwan ROC Joint Quantum Institute and Maryland Center for Fundamental Physics University of Maryland College Park Maryland 20742 USA

In this paper we examine some foundational issues of a class of quantum engines where the system consists of a single quantum parametric oscillator, operating in an Otto cycle consisting of four stages of two alternating phases: the isentropic phase is detached from any bath (thus a closed system) where the natural frequency of the oscillator is changed from one value to another, and the isothermal phase where the system (now rendered open) is put in contact with one or two squeezed baths of different temperatures, whose nonequilibrium dynamics follows the Hu-Paz-Zhang (HPZ) master equation for quantum Brownian motion. The HPZ equation is an exact non-Markovian equation which preserves the positivity of the density operator and is valid for (1) all temperatures, (2) arbitrary spectral density of the bath, and (3) arbitrary coupling strength between the system and the bath. Taking advantage of these properties we examine some key foundational issues of theories of quantum open and squeezed systems for these two phases of the quantum Otto engines. This includes (1) the non-Markovian regimes for non-Ohmic, low-temperature baths, (2) what to expect in nonadiabatic frequency modulations, (3) strong system-bath coupling, as well as (4) the proper junction conditions between these two phases. Our aim here is not to present ways for attaining higher efficiency but to build a more solid theoretical foundation for quantum engines of continuous variables covering a broader range of parameter spaces that we hope are of use for exploring such possibilities.

关键词： Nonequilibrium & irreversible thermodynamics Open quantum systems Quantum master equation Quantum states of light Quantum thermodynamics Nonequilibrium systems Quantum heat engines & refrigerators

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Polarity-triggered anti-Kasha system for high-contrast cell imaging and classification

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Aggregate 2023年第2期4卷 216-226页

作者： Junyi Gong Peifa Wei Junkai Liu Yuncong Chen Zheng Zhao Weijun Zhao Huilin Xie Chao Ma Jacky W.Y.Lam Kam Sing Wong Ying Li Ben Zhong Tang Shenzhen Institute of Aggregate Science and Technology School of Science and EngineeringThe Chinese University of Hong KongShenzhenChina Department of Chemistry Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and ReconstructionInstitute for Advanced StudyState Key Laboratory of Molecular NanoscienceDivision of Life Science and Department of Chemical and Biological EngineeringThe Hong Kong University of Science and TechnologyClear Water BayKowloonChina Institutes of Physical Science and Information Technology Anhui UniversityHefeiChina Department of Physics HKUSTKowloonChina Guangzhou Municipal and Guangdong Provincial Key Laboratory of Molecular Target and Clinical Pharmacology The NMPA and State Key Laboratory of Respiratory DiseaseInnovation Research Center for AIE Pharmaceutical BiologySchool of Pharmaceutical Sciences and the Fifth Affiliated HospitalGuangzhou Medical UniversityGuangzhouChina Center for AIE Research Shenzhen Key Laboratory of Polymer Science and TechnologyGuangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Material Science and EngineeringShenzhen UniversityShenzhenChina Center for Aggregation-Induced Emission SCUT-HKUST Joint Research InstituteState Key Laboratory of Luminescent Materials and DevicesSouth China University of TechnologyGuangzhouChina AIE Institute Guangzhou Development DistrictHuangpuChina

Kasha’s rule,which states that all exciton emissions occur from the lowest excited state and are independent of excitation energy,makes high-energy excitons difficult to use and severely hinders the widespread applications of organic photoluminescent materials in the real *** decades,scientists have tried to break this rule to unleash the power of high-energy excitons,but only minimal progress has been achieved,with no rational guiding principles provided,and few applications *** far,breaking Kasha’s rule has remained a purely academic *** this paper,we introduce a design principle for a purely organic anti-Kasha system and synthesise a series of compounds based on the design *** predicted,these compounds all display evident S_(2) emissions in dilute *** addition,we introduce a highly accurate(over 90%)convolutional neural network as an assistant for the classification of cells using anti-Kasha luminogens,thereby providing a new application direction for anti-Kasha systems.

关键词： anti-Kasha cell classification excited-state dynamics fluorescence

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Achieving a high energy storage density in Ag(Nb,Ta)O_(3) antiferroelectric films via nanograin engineering

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Journal of Advanced Ceramics 2023年第1期12卷 196-206页

作者： Hongbo CHENG Xiao ZHAI Jun OUYANG Limei ZHENG Nengneng LUO Jinpeng LIU Hanfei ZHU Yingying WANG Lanxia HAO Kun WANG Institute of Advanced Energy Materials and Chemistry School of Chemistry and Chemical EngineeringQilu University of Technology(Shandong Academy of Sciences)Jinan 250353China College of Electronic and Optical Engineering Nanjing University of Posts and TelecommunicationsNanjing 210023China School of Physics Shandong UniversityJinan 250100China Guangxi Key Laboratory of Processing for Non-ferrous Metallic and Featured Materials School of ResourcesEnvironment and MaterialsCenter on Nanoenergy ResearchSchool of Physical Science and TechnologyGuangxi UniversityNanning 530004China Key Laboratory for Liquid-Solid Structure Evolution and Processing of Materials(Ministry of Education) School of Materials Science and EngineeringShandong UniversityJinan 250061China Jinan Cigarette Factory China Tobacco Shandong Industrial Co.Ltd.Jinan 250104China

Due to its lead-free composition and a unique double polarization hysteresis loop with a large maximum polarization(Pmax)and a small remnant polarization(Pr),AgNbO_(3)-based antiferroelectrics(AFEs)have attracted extensive research interest for electric energy storage ***,a low dielectric breakdown field(Eb)limits an energy density and its further *** this work,a highly efficient method was proposed to fabricate high-energy-density Ag(Nb,Ta)O_(3) capacitor films on Si substrates,using a two-step process combining radio frequency(RF)-magnetron sputtering at 450℃and post-deposition rapid thermal annealing(RTA).The RTA process at 700℃led to sufficient crystallization of nanograins in the film,hindering their lateral growth by employing short annealing time of 5 *** obtained Ag(Nb,Ta)O_(3) films showed an average grain size(D)of~14 nm(obtained by Debye-Scherrer formula)and a slender room temperature(RT)polarization-electric field(P-E)loop(Pr≈3.8 mC·cm^(−2) and P_(max)≈38 mC·cm^(−2) under an electric field of~3.3 MV·cm^(−1)),the P-E loop corresponding to a high recoverable energy density(W_(rec))of~46.4 J·cm^(−3) and an energy efficiency(η)of~80.3%.Additionally,by analyzing temperature-dependent dielectric property of the film,a significant downshift of the diffused phase transition temperature(T_(M2-M3))was revealed,which indicated the existence of a stable relaxor-like AFE phase near the *** downshift of the T_(M2-M3) could be attributed to a nanograin size and residual tensile strain of the film,and it led to excellent temperature stability(20-240℃)of the energy storage performance of the *** results indicate that the Ag(Nb,Ta)O_(3) film is a promising candidate for electrical energy storage applications.

关键词： antiferroelectrics(AFE) AgNbO_(3) Ag(Nb Ta)O_(3) energy storage film capacitors nanograin engineering

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Inferring phase transitions and critical exponents from limited observations with Thermodynamic Maps

arXiv

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arXiv 2023年

作者： Herron, Lukas Mondal, Kinjal Schneekloth, John S. Tiwary, Pratyush Biophysics Program Institute for Physical Science and Technology University of Maryland College ParkMD20742 United States Chemical Biology Laboratory National Cancer Institute FrederickMD21702 United States Department of Chemistry and Biochemistry Institute for Physical Science and Technology University of Maryland College ParkMD20742 United States

Phase transitions are ubiquitous across life, yet hard to quantify and describe accurately. In this work, we develop an approach for characterizing generic attributes of phase transitions from very limited observations made deep within different phases' domains of stability. Our approach is called Thermodynamic Maps, which combines statistical mechanics and molecular simulations with score-based generative models. Thermodynamic Maps enable learning the temperature dependence of arbitrary thermodynamic observables across a wide range of temperatures. We show its usefulness by calculating phase transition attributes such as melting temperature, temperature-dependent heat capacities, and critical exponents. For instance, we demonstrate the ability of thermodynamic maps to infer the ferromagnetic phase transition of the Ising model, including temperature-dependent heat capacity and critical exponents, despite never having seen samples from the transition region. In addition, we efficiently characterize the temperature-dependent conformational ensemble and compute melting curves of the two RNA systems GCAA tetraloop and HIV-TAR, which are notoriously hard to sample due to glassy-like landscapes. © 2023, CC BY.

关键词： Specific heat

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A hierarchical heterostructure of CdS QDs confined on 3D ZnIn_(2)S_(4) with boosted charge transfer for photocatalytic CO_(2) reduction

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Nano Research 2021年第1期14卷 81-90页

作者： Zezhou Zhu Xiaoxia Li Yunteng Qu Fangyao Zhou Zhiyuan Wang Wenyu Wang Changming Zhao Huijuan Wang Liqiang Li Yagang Yao Qun Zhang Yuen Wu School of Nano-Tech and Nano-Bionics Hefei National Laboratory for Physical Sciences at the MicroscaleCollaborative Innovation Center of Chemistry for Energy Materials(iChEM)School of Chemistry and Materials Scienceand National Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei 230026China Hefei National Laboratory for Physical Sciences at the Microscale Synergetic Innovation Center of Quantum Information and Quantum PhysicsDepartment of Chemical PhysicsUniversity of Science and Technology of ChinaHefei 230026China Division of Advanced Nanomaterials Suzhou Institute of Nano-tech and Nano-bionicsChinese Academy of SciencesSuzhou 215123China Center for Micro and Nanoscale Research and Fabrication University of Science and Technology of ChinaHefei 230026China

Metal sulfide based materials as photocatalysts for energy conversion are essential to produce value-added chemical fuels,but their intrinsically slow carrier dynamics and low activity are yet to be ***,we developed a unique heterogeneously nanostructured ZnIn_(2)S_(4)-CdS heterostructure that involves zero-dimensional(0D)CdS quantum dots uniformly confined on three-dimensional(3D)ZnIn_(2)S_(4)nanoflowers,which achieves an excellent catalytic performance of CO_(2) photoconversion under visible-light *** obtained hierarchical heterostructure can significantly enhance the light harvesting,shorten the migration distance of carriers,and obviously accelerate the transport of *** evidenced by the ultrafast transient absorption spectroscopy,the formed interface can effectively facilitate charge separation and *** work opens up a new avenue to carefully design the elaborate heterostructures for achieving optimal charge separation efficiency by lowering interfacial kinetic barriers and energy losses at the interface.

关键词： photocatalysis CO_(2)reduction charge transfer hierarchical heterostructure

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Glass Transition in Monolayers of Rough Colloidal Ellipsoids

arXiv

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arXiv 2024年

作者： Liang, Jian Feng, Xuan Zheng, Ning Wang, Huaguang Ni, Ran Zhang, Zexin College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou215123 China School of Chemistry Chemical Engineering and Biotechnology Nanyang Technological University 62 Nanyang Drive 637459 Singapore School of Physics Beijing Institute of Technology Beijing100081 China Institute for Advanced Study Center for Soft Condensed Matter Physics and Interdisciplinary Research School of Physical Science and Technology Soochow University Suzhou215006 China

Structure-dynamics correlation is one of the major ongoing debates in the glass transition, although a number of structural features have been found connected to the dynamic heterogeneity in different glass-forming colloidal systems. Here using colloidal experiments combined with coarse-grained molecular dynamics simulations, we investigate the glass transition in monolayers of rough colloidal ellipsoids. Compared with smooth colloidal ellipsoids, the surface roughness of ellipsoids is found to significantly change the nature of glass transition. In particular, we find that the surface roughness induced by coating only a few small hemispheres on the ellipsoids can eliminate the existence of orientational glass and the two-step glass transition found in monolayers of smooth ellipsoids. This is due to the surface roughness-induced coupling between the translational and rotational degrees of freedom in colloidal ellipsoids, which also destroys the structure-dynamics correlation found in glass-forming suspensions of colloidal ellipsoids. Our results not only suggest a new way of using surface roughness to manipulate the glass transition in colloidal systems, but also highlight the importance of detailed particle shape on the glass transition and structure-dynamics correlation in suspensions of anisotropic colloids. Copyright © 2024, The Authors. All rights reserved.

关键词： Glass transition

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Proton-transfer-induced in situ defect passivation for highly efficient wide-bandgap inverted perovskite solar cells

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InfoMat 2022年第6期4卷 121-128页

作者： Zhimin Fang Lingbo Jia Nan Yan Xiaofen Jiang Xiaodong Ren Shangfeng Yang Shengzhong(Frank)Liu Key Laboratory of Applied Surface and Colloid Chemistry Ministry of Education Shaanxi Key Laboratory for Advanced Energy DevicesShaanxi Engineering Lab for Advanced Energy Technology School of Materials Science and EngineeringShaanxi Normal UniversityXi'anChina Hefei National Laboratory for Physical Sciences at Microscale CAS Key Laboratory of Materials for Energy ConversionAnhui Laboratory of Advanced Photon Science and TechnologyDepartment of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefeiChina Dalian National Laboratory for Clean Energy iChEM Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalianChina

Wide-bandgap(≥1.68 eV)inverted perovskite solar cells(PSCs)have been recognized as promising top component cells on the commercial crystalline silicon cell to surpass its Shockley-Queisser efficiency ***,the power conversion efficiency(PCE)is dramatically limited by the huge open-circuit voltage(V_(OC))***,we propose a proton-transfer-induced in situ defect passivation strategy to reduce the nonradiative recombination to minimize the VOC ***,a liquid-form neutral amine,3,4,5-trifluorobenzylamine(TFBA)was added into ethyl acetate(EA)as anti-solvent for the film preparation,which induces proton-transfer from the formamidinium(FA)and methylammonium(MA)in the perovskite precursors to the *** protonated TFBA exhibits a gradient distribution near the surface of the perovskite film,achieving in situ defect *** a result,TFBA-based 1.68 eV-bandgap inverted PSCs afforded a PCE of 20.39%,one of the highest for cells with this ***,due to the strong interaction between TFBA and the perovskite film,the mixed-halide perovskites demonstrate much better *** findings offer an effective strategy to passivate defects in PSCs.

关键词： defect efficiency passivation perovskite solar cell wide-bandgap

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Growth,coalescence,and etching of two-dimensional overlayers on metals modulated by near-surface Ar nanobubbles

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Nano Research 2022年第3期15卷 2706-2714页

作者： Wei Wei Jiaqi Pan Haiping Lin Chanan Euaruksakul Zhiyun Li Rong Huang Li Wang Zhujun Wang Qiang Fu Yi Cui Vacuum Interconnected Nanotech Workstation Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123China Institute of Functional Nano&Soft Materials(FUNSOM) Soochow UniversitySuzhou 215123China Synchrotron Light Research Institute Nakhon Ratchasima 30000Thailand School of Physical Science and Technology Shanghai Tech UniversityShanghai 200031China Scientific Center for Optical and Electron Microscopy ETH Zürich8093 ZürichSwitzerland State Key Laboratory of Catalysis iChEMDalian Institute of Chemical Physicsthe Chinese Academy of SciencesDalian 116023China

The synthesis of high-quality ultrathin overlayers is critically dependent on the surface structure of substrates,especially involving the overlayer–substrate *** using in situ surface measurements,we demonstrate that the overlayer–substrate interaction can be tuned by doping near-surface Ar *** interfacial coupling strength significantly decreases with near-surface Ar nanobubbles,accompanying by an“anisotropic to isotropic”growth *** the substrate containing near-surface Ar,the growth front crosses entire surface atomic steps in both uphill and downhill directions with no difference,and thus,the morphology of the two-dimensional(2D)overlayer exhibits a ***,the round-shaped 2D overlayers coalesce seamlessly with a growth acceleration in the approaching direction,which is barely observed in the synthesis of 2D *** can be attributed to the immigration lifetime and diffusion rate of growth species,which depends on the overlayer–substrate interaction and the surface ***,the“round to hexagon”morphological transition is achieved by etching-regrowth,revealing the inherent growth kinetics under quasi-freestanding *** findings provide a novel promising way to modulate the growth,coalescence,and etching dynamics of 2D materials on solid surfaces by adjusting the strength of overlayer–substrate interaction,which contributes to optimization of large-scale production of 2D material crystals.

关键词： two dimensional materials overlayer–substrate interaction near-surface Ar nanobubbles evolution behavior surface dynamics

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Catalytic conversion of lignocellulosic biomass into chemicals and fuels

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Green Energy & Environment 2023年第1期8卷 10-114页

作者： Weiping Deng Yunchao Feng Jie Fu Haiwei Guo Yong Guo Buxing Han Zhicheng Jiang Lingzhao Kong Changzhi Li Haichao Liu Phuc T.T.Nguyen Puning Ren Feng Wang Shuai Wang Yanqin Wang Ye Wang Sie Shing Wong Kai Yan Ning Yan Xiaofei Yang Yuanbao Zhang Zhanrong Zhang Xianhai Zeng Hui Zhou State Key Laboratory for Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy MaterialsNational Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Estersand College of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China Fujian Engineering and Research Center of Clean and High-valued Technologies for Biomass Xiamen Key Laboratory of High-valued Utilization of BiomassCollege of EnergyXiamen University361102China Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou310027China Institute of Zhejiang University-Quzhou 78 Jiuhua Boulevard NorthQuzhou324000China School of Energy and Environmental Engineering Hebei University of TechnologyTianjin300401China Shanghai Key Laboratory of Functional Materials Chemistry Research Institute of Industrial CatalysisSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai200237China Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and ThermodynamicsCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing100190China Department of Biomass Science and Engineering Sichuan UniversityChengdu610065China CAS Key Laboratory of Low-carbon Conversion Science and Engineering Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai201210China University of Chinese Academy of Sciences Beijing100049China CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023China Beijing National Laboratory for Molecular Sciences College of Chemistry and Molecular EngineeringPeking UniversityBeijing100871China Department of Chemical and Biomolecular Engineering National University of Singapore4 Engineering Drive 4Singapore117585Singapore Sta

In the search of alternative resources to make commodity chemicals and transportation fuels for a low carbon future,lignocellulosic biomass with over 180-billion-ton annual production rate has been identified as a promising *** review focuses on the state-of-the-art catalytic transformation of lignocellulosic biomass into value-added chemicals and *** a brief introduction on the structure,major resources and pretreatment methods of lignocellulosic biomass,the catalytic conversion of three main components,i.e.,cellulose,hemicellulose and lignin,into various compounds are comprehensively *** in separate steps or in one-pot,cellulose and hemicellulose are hydrolyzed into sugars and upgraded into oxygen-containing chemicals such as 5-HMF,furfural,polyols,and organic acids,or even nitrogen-containing chemicals such as amino *** the other hand,lignin is first depolymerized into phenols,catechols,guaiacols,aldehydes and ketones,and then further transformed into hydrocarbon fuels,bioplastic precursors and bioactive *** review then introduces the transformations of whole biomass via catalytic gasification,catalytic pyrolysis,as well as emerging ***,opportunities,challenges and prospective of woody biomass valorization are highlighted.

关键词： Lignocelullose Biomass Catalytic conversion Biofuels Renewable chemicals

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