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SSRN 2023年

作者： Acuna-Yeomans, Esteban Gutiérrez-Sevillano, J.J. Dubbeldam, David Calero, Sofia Materials Simulation and Modelling Department of Applied Physics and Science Education Eindhoven University of Technology Eindhoven5600 MB Netherlands Department of Physical Chemical and Natural Systems Universidad Pablo de Olavide Ctra. Utrera Km. 1 SevilleES-41013 Spain Van’t Hoff Institute for Molecular Sciences University of Amsterdam Science Park 904 Amsterdam1098XH Netherlands Eindhoven University of Technology P.O. Box 513 Eindhoven5600 MB Netherlands

In this work, we computationally investigate the impact of the distribution of linker vacancies on the relative stability of defected UiO-66 structures. Analysis of a significant number of defected structures reveals that higher defect numbers correlate with lower stability, but variations in missing linker distribution and orientation contribute to widely differing amorphization pressures. Our results suggest that structures with more evenly distributed vacancies exhibit a positive linear relationship between amorphization pressure and bulk modulus. Furthermore, we found structures with a disproportionate number of missing linkers with the same orientation and structures where a large volume of the framework remains pristine, display outlier behavior in this respect. Evaluation of anisotropic elastic moduli uncovers directional instability in structures with a high number of vacancies with the same orientation. These findings have important implications for designing and optimizing UiO-66-based materials, aiding in defect configuration selection for specific applications. © 2023, The Authors. All rights reserved.

关键词： Mechanical stability

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In-medium screening effects for the Galactic halo and solar-reflected dark matter detection in semiconductor targets

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physical Review D 2021年第9期104卷 096001-096001页

作者： Zheng-Liang Liang Chongjie Mo Ping Zhang College of Mathematics and Physics Beijing University of Chemical Technology Beijing 100029 China Beijing Computational Science Research Center Beijing 100193 China School of Physics and Physical Engineering Qufu Normal University Qufu 273165 China Institute of Applied Physics and Computational Mathematics Beijing 100088 China

Recently, the importance of the electronic many-body effect in the dark matter (DM) detection has been recognized, and a coherent formulation of the DM-electron scattering in terms of the dielectric response of the target material has been well established in literatures. In this paper, we put relevant formulas into practical density functional theory (DFT) estimation of the excitation event rates for the diamond and silicon semiconductor targets. Moreover, we compare the event rates calculated from the energy loss functions with and without the local field effects. For a consistency check of this numerical method, we also compare the differential spectrum and detection reach of the silicon target with those computed with the GPAW code. It turns out that these DFT approaches are quite consistent and robust. As an interesting extension, we also investigate the in-medium effect on the detection of the solar-reflected DM flux in silicon-based detectors, where the screening effect is found to be less remarkable than on detection of the Galactic DM, due to the high energies of the reflected DM particles.

关键词： Particle dark matter Ab initio calculations Density functional theory Solid-state detectors

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Long-Cyclic and High-Energy-Density Fe-Metal Batteries with Smart Anode/Cathode-Free Design and Electrolyte Engineering

SSRN

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SSRN 2023年

作者： Jiang, Jian Zheng, Jiajie Chai, Shibo Wang, Yanlong Zhu, Jianhui Xu, Maowen School of Physical Science and Technology Chongqing Key Laboratory of Micro & Nano Structure Optoelectronics Southwest University No.2 Tiansheng Road BeiBei District Chongqing400715 China School of Materials and Energy Chongqing Key Lab for Advanced Materials and Clean Energies of Technologies Southwest University No. 2 Tiansheng Road BeiBei District Chongqing400715 China Key Laboratory of Chemical Lasers Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian116023 China

Rechargeable Fe-metal aqueous batteries (ABs) have become thriving due to their great theoretical capacity, low cost and salient environmental benignity. However, their further development is impeded by poor cyclic stability of ferruginous cathodes, and low specific energy due to limited utilization ratio for Fe metal anode. To overcome above constrains, we herein propose to construct unique Fe-metal ABs free of both anode and cathode. Unlike traditional Fe-related ABs, they are only configured by symmetric carbonaceous current collectors among which ferrous ions shuttle upon charge/discharge procedures. Besides, the commonly used additives (NH4Cl or MnSO4) are tried to mediate ferrous electrolytes, endowing the nominal anode with elevated Fe plating/stripping efficiency (Max.: ~96.4% at 10 mA/cm2), enhanced gravimetric capacity and prolonged cyclability over 1000 cycles. As for the nominal cathode, the reversible deposition/dissolution of gel-like ferric species are governed by intrinsic surface properties for carbon hosts. As evaluated, our packed pouch cells deliver far superior CE (Max.: 95.3%), capacity retention (94.4% after 1000 times of deep cycles) and energy density (41.86 Wh/kg) to conventional counterparts. This paradigm engineering work opens up a new avenue to build better batteries, not only for Fe-metal ABs but also applicable to other charge-storage cell systems. © 2023, The Authors. All rights reserved.

关键词： Cathodes

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Ground state of the S=1/2 pyrochlore Heisenberg antiferromagnet: A quantum spin liquid emergent from dimensional reduction

arXiv

引用

arXiv 2023年

作者： Pohle, Rico Yamaji, Youhei Imada, Masatoshi Waseda Research Institute for Science and Engineering Waseda University 3-4-1 Okubo Shinjuku-ku Tokyo169-8555 Japan Department of Applied Physics University of Tokyo Hongo Bunkyo-ku Tokyo113-8656 Japan Graduate School of Science and Technology Keio University Yokohama223-8522 Japan Namiki Ibaraki Tsukuba305-0044 Japan Toyota Physical and Chemical Research Institute Yokomichi Aichi Nagakute480-1192 Japan Sophia University Kioicho Chiyoda-ku Tokyo Japan

The quantum antiferromagnet on the pyrochlore lattice offers an archetypal frustrated system, which potentially realizes a quantum spin liquid characterized by the absence of standard spontaneous symmetry breaking even at zero temperature, unusually as an isotropic 3D system. Despite tremendous progress in the literature, however, the nature of the ground state of the fully quantum-mechanical spin Hamiltonian on the pyrochlore lattice still remains elusive. Here, we show that an unconventional type of quantum spin liquid is born out from the pyrochlore system after the self-organized dimensional reduction leading to confined states in 2D layers. This conclusion is obtained from state-of-the-art variational Monte Carlo (VMC) simulations at zero temperature. Quantum spin liquids triggered by the emergent dimensional reduction is an unexplored route of the spin-liquid formation. The dimensional reduction from 3D to 2D is a consequence of a conventional spontaneous symmetry breaking, while the resultant decoupling of layers enables the emergence of a 2D quantum spin liquid that is adiabatically disconnected from trivial product states and exhibits strong quantum entanglement. The stabilized quantum spin liquid exhibits an algebraic decay of correlations and vanishing excitation gap in the thermodynamic limit. The wave-function structure supports the fractionalization of the spin into spinons. This spin-liquid ground state persists in the presence of spin-orbit interactions, which expands the possibilities of realizing quantum spin liquids in real pyrochlore-structured materials. Copyright © 2023, The Authors. All rights reserved.

关键词： Ground state

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Nucleic Acid Nanoprobes for Biosensor Development in Complex Matrices

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chemical Research in Chinese Universities 2020年第2期36卷 185-193页

作者： DENG Mengying LI Min MAO Xiuliai LI Fan ZUO Xiaolei Division of Physical Biology CAS Key Laboratory of Interfacial Physics and TechnologyShanghai Synchrotron Radiation Facility(SSRF)Shanghai Institute of Applied PhysicsChinese Academy of SciencesShanghai 201800P R.China University of Chinese Academy of Science Beijing 100049P.R.China Institute of Molecular Medicine Renji HospitalSchool of Medicine and School of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200127P.R.China

Nucleic acid probes in living organisms play an essential role in therapeutics and *** the imaging and sensing of nucleic acid probes in complex biological matrices,a variety of diseases-related biological process,pathogenic process,or pharmacological responses to a therapeutic intervention have been ***,a critical challenge of nucleic acid probes applied in complex matrices lies in enhancing the stability of nucleic acid probes,especially when it suffers from nuclease degradation and protein *** order to enhance the application of nucleic acid nanoprobes in complex matrices,great efforts have been devoted to improving the stability of probes operated in complex media,including construction of nucleic acid nanoprobes with nuclease resistance and protein adsorption resistance,sample pretreatment,anti-biofouling and signal *** this review,we aim to summarize recent advances in the stability of nucleic acid nanoprobes in complex matrices,including the methods of enhancing the stability of probes or signals,and the application of nucleic acid nanoprobes for disease diagnosis.

关键词： Nuclease-resistance Complex matrix Nucleic acid probe Stability

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Perovskite Solar Cells toward Eco-Friendly Printing

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Research 2021年第1期2021卷 586-596页

作者： Xiaoming Chang Yuanyuan Fan Kui Zhao Junjie Fang Dongle Liu Ming-Chun Tang Dounya Barrit Detlef-MSmilgies Ruipeng Li Jing Lu Jianbo Li Tinghuan Yang Aram Amassian Zicheng Ding Yonghua Chen Shengzhong(Frank)Liu Wei Huang Key Laboratory of Applied Surface and Colloid Chemistry Ministry of EducationShaanxi Key Laboratory for Advanced Energy DevicesShaanxi Engineering Lab for Advanced Energy TechnologySchool of Materials Science and EngineeringShaanxi Normal UniversityXi’an 710119China King Abdullah University of Science and Technology(KAUST) KAUST Solar Center(KSC)and Physical Science and Engineering Division(PSE)Thuwal 23955-6900Saudi Arabia Cornell High Energy Synchrotron Source Cornell UniversityIthacaNY 14850USA NSLS II Brookhaven National LabUpton New York 11973USA Department of Materials Science and Engineering and Carbon and Organic Electronics Laboratories(ORaCEL)North Carolina State UniversityRaleighNC 27695USA Key Laboratory of Flexible Electronics(KLOFE)&Institute of Advanced Materials(IAM) Nanjing Tech University(NanjingTech)Nanjing211800 JiangsuChina Dalian National Laboratory for Clean Energy iChEMDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Frontiers Science Center for Flexible Electronics Shaanxi Institute of Flexible Electronics(SIFE)and Xi’an Institute of Biomedical Materials&EngineeringNorthwestern Polytechnical University(NPU)127 West Youyi RoadXi’an710072 ShaanxiChina

Eco-friendly printing is important for mass manufacturing of thin-film photovoltaic(PV)devices to preserve human safety and the environment and to reduce energy consumption and capital ***,it is challenging for perovskite PVs due to the lack of eco-friendly solvents for ambient fast *** this study,we demonstrate for the first time an eco-friendly printing concept for high-performance perovskite solar *** the perovskite and charge transport layers were fabricated from eco-friendly solvents via scalable fast blade coating under ambient *** perovskite dynamic crystallization during blade coating investigated using in situ grazing incidence wide-angle X-ray scattering(GIWAXS)reveals a long sol-gel window prior to phase transformation and a strong interaction between the precursors and the eco-friendly *** insights enable the achievement of high quality coatings for both the perovskite and charge transport layers by controlling film formation during scalable *** excellent optoelectronic properties of these coatings translate to a power conversion efficiency of 18.26%for eco-friendly printed solar cells,which is on par with the conventional devices fabricated via spin coating from toxic solvents under inert *** eco-friendly printing paradigm presented in this work paves the way for future green and highthroughput fabrication on an industrial scale for perovskite PVs.

关键词： coating printing blade

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Crystal-plane effects of anatase TiO₂ on the selective hydrogenation of crotonaldehyde over Ir/TiO₂ catalysts

引用

Journal of Catalysis 2021年 395卷 10-22页

作者： Jia, Aiping Zhang, Yunshang Song, Tongyang Zhang, Zhenhua Tang, Cen Hu, Yiming Zheng, Wanbin Luo, Mengfei Lu, Jiqing Huang, Weixin Hefei National Laboratory for Physical Sciences at the Microscale Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes CAS Key Laboratory of Materials for Energy Conversion and Department of Chemical Physics University of Science and Technology of China Hefei 230026 China Key Laboratory of the Ministry of Education for Advanced Catalysis Materials Institute of Physical Chemistry Zhejiang Normal University Jinhua 321004 China Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular Engineering East China Normal University Shanghai 200062 China Dalian National Laboratory for Clean Energy Dalian 116023 China

Supported Ir/TiO2 catalysts with the anatase TiO2 nanocrystals exposing {1 0 1}, {1 0 0} and {0 0 1} planes were tested for selective hydrogenation of crotonaldehyde. The Ir/TiO2-{1 0 1} catalyst dominantly exposing {... 详细信息

Supported Ir/TiO₂ catalysts with the anatase TiO₂ nanocrystals exposing {1 0 1}, {1 0 0} and {0 0 1} planes were tested for selective hydrogenation of crotonaldehyde. The Ir/TiO₂-{1 0 1} catalyst dominantly exposing {1 0 1} plane gave a initial reaction rate of 166.1 μmol g_Ir^-1 s⁻¹ at 80 °C and a turnover frequency of crotyl alcohol formation of 0.022 s⁻¹, which is 5 and 7 times respectively higher than those obtained on the Ir/TiO₂-{0 0 1} catalyst dominantly exposing {0 0 1} plane even though they have similar Ir particle sizes (ca. 1.3 nm). The reaction behaviors were related to the surface oxygen vacancy, which served as surface acid sites and provide adsorption sites for C[dbnd]O bond in the CRAL molecule. Therefore, the higher concentration of oxygen vacancy in the Ir/TiO₂-{1 0 1} accounted for the improved performance compared to the Ir/TiO₂-{0 0 1}. However, strong adsorption of crotonaldehyde and/or products on the catalyst surface, as well as the CO poisoning via decarbonylation of crotonaldehyde, were the main reasons for the catalyst deactivation. © 2020 Elsevier Inc.

关键词： Crystal plane effect Defects Hydrogenation Ir/TiO2 Reaction mechanism α, β - unsaturated aldehyde

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Joint Observation of the Galactic Center with MAGIC and CTA-LST-1 38

Joint Observation of the Galactic Center with MAGIC and CTA-...

引用

38th International Cosmic Ray Conference, ICRC 2023

作者： Abe, Shotaro Berti, Alessio Di Pierro, Federico López-Coto, Rubén Moralejo, Abelardo Ohtani, Yoshiki Sitarek, Julian Strzys, Marcel Suda, Yusuke Vovk, Ievgen Abe, H. Abe, K. Abe, S. Abhir, J. Acciari, V.A. Aguasca-Cabot, A. Agudo, I. Alvarez Crespo, N. Aniello, T. Ansoldi, S. Antonelli, L.A. Aramo, C. Arbet-Engels, A. Cornelia, A. Artero, M. Asano, K. Aubert, P. Baack, D. Babić, A. Baktash, A. Bamba, A. Baquero Larriva, A. Baroncelli, L. Barres de Almeida, U. Barrio, J.A. Batkovic, I. Baxter, J. Becerra González, J. Bednarek, W. Bernardini, E. Bernardos, M.I. Bernete Medrano, J. Berti, A. Besenrieder, J. Bhattacharjee, P. Biederbeck, N. Bigongiari, C. Biland, A. Bissaldi, E. Blanch, O. Bonnoli, G. Bordas, P. Bošnjak, Ž. Bulgarelli, A. Burelli, I. Burmistrov, L. Buscemi, M. Busetto, G. Campoy-Ordaz, A. Cardillo, M. Caroff, S. Carosi, A. Carosi, R. Carrasco, M.S. Carretero-Castrillo, M. Cassol, F. Castro-Tirado, A.J. Cauz, D. Cerasole, D. Ceribella, G. Chai, Y. Cheng, K. Chiavassa, A. Chikawa, M. Chilingarian, A. Chytka, L. Cifuentes, A. Cikota, S. Colombo, E. Contreras, J.L. Cortina, J. Costantini, H. Covino, S. D’Amico, G. Dalchenko, M. D’Elia, V. Da Vela, P. Dazzi, F. De Angelis, A. de Bony de Lavergne, M. De Lotto, B. De Lucia, M. de Menezes, R. Del Peral, L. Deleglise, G. Delfino, M. Delgado, C. Delgado Mengual, J. della Volpe, D. Dellaiera, M. Del Popolo, A. Depaoli, D. Di Piano, A. Di Pierro, F. Di Pilato, A. Di Tria, R. Di Venere, L. Díaz, C. Dominik, R.M. Dominis Prester, D. Donini, A. Dorner, D. Doro, M. Eisenberger, L. Elsässer, D. Emery, G. Escudero, J. Fallah Ramazani, V. Fariña, L. Fattorini, A. Ferrara, G. Ferrarotto, F. Fiasson, A. Foffano, L. Font, L. Freixas Coromina, L. Fröse, S. Fukami, S. Fukazawa, Y. Garcia, E. Garcia López, R. Garczarczyk, M. Gasbarra, C. Gasparrini, D. Gasparyan, S. Gaug, M. Geyer, D. Giesbrecht Paiva, J. Giglietto, N. Giordano, F. Gliwny, P. Godinovic, N. Grau, R. Green, J. Green, D. Gunji, S. Günther, P. Hackfeld, J. Hadasch, D. Hahn, A. Institute for Cosmic Ray Research Kashiwa-no-ha 5-1-5 Kashiwa-shi Chiba Japan Max-Planck-Institut für Physik Föhringer Ring 6 München80805 Germany INFN Sezione di Torino Via P. Giuria 1 Torino10125 Italy Instituto de Astrofísica de Andalucía-CSIC Glorieta de la Astronomía s/n Granada18008 Spain The Barcelona Institute of Science and Technology Campus UAB Bellaterra Barcelona08193 Spain Faculty of Physics and Applied Informatics University of Lodz ul. Pomorska 149-153 Lodz90-236 Poland Physics Program Graduate School of Advanced Science and Engineering Hiroshima University Hiroshima739-8526 Japan Institute for Cosmic Ray Research University of Tokyo Japan Department of Physics Tokai University Japan ETH Zürich Switzerland Instituto de Astrofísica de Canarias Departamento de Astrofísica Universidad de La Laguna Spain Departament de Física Quàntica i Astrofísica Institut de Ciències del Cosmos Universitat de Barcelona IEEC-UB Spain EMFTEL department IPARCOS Universidad Complutense de Madrid Spain Italy INFN Sezione di Trieste Università degli Studi di Udine Italy Italy INAF Osservatorio Astronomico di Roma Italy INFN Sezione di Napoli Italy INFN Sezione di Padova Università degli Studi di Padova Italy LAPP Univ. Grenoble Alpes Univ. Savoie Mont Blanc CNRS-IN2P3 Annecy France Department of Physics TU Dortmund University Germany Croatia Universität Hamburg Institut für Experimentalphysik Germany Graduate School of Science University of Tokyo Japan Universidad del Azuay Ecuador INAF Osservatorio di Astrofisica e Scienza dello spazio di Bologna Italy Centro Brasileiro de Pesquisas Físicas Brazil CIEMAT Spain INFN Sezione di Bari Politecnico di Bari Italy INAF Osservatorio Astronomico di Brera Italy University of Geneva Département de physique nucléaire et corpusculaire Switzerland INFN Sezione di Catania Italy Departament de Física CERES-IEEC Universitat Autónoma de Barcelona Spain Italy Università di Pisa INFN Pisa Italy Aix Mars

MAGIC is a system of two Imaging Atmospheric Cherenkov Telescopes (IACTs), designed to detect very-high-energy gamma rays, and is operating in stereoscopic mode since 2009 at the Observatorio del Roque de Los Muchachos in La Palma, Spain. In 2018, the prototype IACT of the Large-Sized Telescope (LST-1) for the Cherenkov Telescope Array, a next-generation ground-based gamma-ray observatory, was inaugurated at the same site, at a distance of approximately 100 meters from the MAGIC telescopes. Using joint observations between MAGIC and LST-1, we developed a dedicated analysis pipeline and established the threefold telescope system via software, achieving the highest sensitivity in the northern hemisphere. Based on this enhanced performance, MAGIC and LST-1 have been jointly and regularly observing the Galactic Center, a region of paramount importance and complexity for IACTs. In particular, the gamma-ray emission from the dynamical center of the Milky Way is under debate. Although previous measurements suggested that a supermassive black hole Sagittarius A* plays a primary role, its radiation mechanism remains unclear, mainly due to limited angular resolution and sensitivity. The enhanced sensitivity in our novel approach is thus expected to provide new insights into the question. We here present the current status of the data analysis for the Galactic Center joint MAGIC and LST-1 observations. © Copyright owned by the author(s) under the terms of the Creative Commons.

关键词： Cosmology

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Molecular-Scale Insights into the Heterogeneous Interactions Between an m-Terphenyl Isocyanide Ligand and Noble Metal Nanoparticles

arXiv

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arXiv 2024年

作者： Bi, Liya Wang, Yufei Wang, Zhe Do, Alexandria Fuqua, Alexander Balto, Krista P. Zhang, Yanning Figueroa, Joshua S. Pascal, Tod A. Tao, Andrea R. Li, Shaowei Department of Chemistry and Biochemistry University of California San DiegoCA92093-0309 United States Program in Materials Science and Engineering University of California San DiegoCA92093-0418 United States Aiiso Department of Chemical and Nano Engineering University of California San DiegoCA92093-0448 United States Department of Physics and Astronomy University of California IrvineCA92697-4575 United States Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China Chengdu611731 China

The structural and chemical properties of metal nanoparticles are often dictated by their interactions with molecular ligand shells. These interactions are highly material-specific and can vary significantly even among elements within the same group or materials with similar crystal structure. Precise characterization of ligand-metal interactions is crucial for the rational design of ligands and the functionalization of nanoparticles. In this study, we found that the ligation behavior with an m-terphenyl isocyanide molecule differs significantly between Au and Ag nanoparticles, with distinct ligand extraction efficiencies and size dependencies. Surface-enhanced Raman spectroscopy measurements revealed unique enhancement factors for two molecular vibrational modes between two metal surfaces, indicating different ligand binding geometries. Molecular-level characterization using scanning tunneling microscopy allowed us to directly visualize these variations between Ag and Au surfaces, which we assign as two distinct binding mechanisms. This molecular-scale visualization provides clear insights into the different ligand-metal interactions, as well as the chemical behavior and spectroscopic characteristics of isocyanide-functionalized nanoparticles. © 2024, CC BY.

关键词： Ligands

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Mn-corrolazine-based 2D-nanocatalytic material with single Mn atoms for catalytic oxidation of alkane to alcohol

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Chinese Journal of Catalysis 2021年第6期42卷 1030-1039页

作者： Chun Zhu Jin-Xia Liang Yang Meng Jian Lin Zexing Cao School of Chemistry and Chemical Engineering Guizhou UniversityGuiyang 550025GuizhouChina Guizhou Provincial Key Laboratory of Computational Nano-Material Science Guizhou Education UniversityGuiyang 550018GuizhouChina CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina State Key Laboratory of Physical Chemistry of Solid Surfaces and Fujian Provincial Key Laboratory of Theoretical and Computational Chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 360015FujianChina

Heterogenization of organic-macrocyclic metal catalysts is one of the simplest and most efficient methods for effective separation of products and cyclic application of a *** using an environmentally friendly Mn-corrolazine catalyst as the building unit,which can directly oxidize organic substrates under oxygen atmosphere and mild conditions,we theoretically constructed a novel two-dimensional(2D)Mn-corrolazine nanocatalytic material with high catalytic *** this material,each Mn atom maintains its electronic configuration in the monomer and can directly activate O2 as the single-atom catalyst(SAC)center to form a radical-like[Mn]-O-O under mild visible-light irradiation *** newly generated[Mn]–O–O can efficiently and selectively oxidize C–H bonds to form alcohol species through H-abstraction and the rebound ***,the catalytic reaction is easily regulated by an external electric field along its intrinsic Mn–O–O reaction *** current study provides a theoretical foundation for further experimental studies and practical applications of the Mn-corrolazine-based SAC.

关键词： Single-atom catalyst Heterogenization Two-dimensional nanomaterials First-principles calculations C–H bond activation

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