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Photo-and Electrocatalytic CO_(2)Reduction Based on Stable Lead-Free Perovskite Cs2PdBr6

Energy & Environmental Materials 2023年第5期6卷 364-371页

作者： Daofu Wu Cheng Wang Benjun Huo Ke Hu Xinchun Mao Zhigang Geng Qiang Huang Wenxia Zhang Jie Zeng Xiaosheng Tang Key Laboratory of Optoelectronic Technology&Systems(Ministry of Education) College of Optoelectronic EngineeringChongqing UniversityChongqing 400044China Hefei National Laboratory for Physical Sciences at the Microscale CAS Key Laboratory of Strongly-Coupled Quantum Matter PhysicsKey Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education InstitutesDepartment of Chemical PhysicsUniversity of Science and Technology of ChinaHefei230026China College of Optoelectronic Engineering Chongqing University of Posts and TelecommunicationsChongqing 400065China School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001China Department of Chemistry Shandong UniversityWeihai 264200China Institute of Materials Chinese Academy of Engineering PhysicsJiangyou 621908China

All-inorganic lead-free palladium(Pd)halogen perovskites with prominent optoelectronic properties provide admirable potential for selective photo-and electroreduction of CO_(2).But it remains unachieved for effectively converting the CO_(2)to CO with high selectivity on Pd-based perovskites driven by solar light or ***,high-quality Cs_(2)PdBr_(6)microcrystals and nanocrystals were synthesized through a facile antisolvent *** all the reported pure-phase perovskites,the Cs_(2)PdBr_(6)nanocrystals synthesized at 50℃performed the highest effectiveness on CO_(2)to CO conversion generating 73.8μmol g^(-1)of CO yield with 100%selectivity under visible light illumination(λ>420 nm)for 3 ***,for the first time,we report a new application of lead-free perovskites,in which they are applied to electrocatalysis of CO_(2)reduction ***,they showed significant electrocatalytic activity(Faradaic yield:78%for CO)and operation stability(10 h).And the surface reaction intermediates were dynamically monitored and precisely unraveled according to the in situ diffuse reflectance infrared Fourier transform spectra *** combination with the density functional theory calculation,the reaction mechanism and pathways were *** work not only provides significant strategies to enhance the photocatalytic performance of perovskites,but also shows excellent potential for their application in electrocatalysis.

关键词： CO_(2)reduction crystallinity lead-free perovskites morphology photocatalysis reaction mechanism

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Large-eddy simulation of Rayleigh-Bénard convection at extreme Rayleigh numbers

arXiv

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arXiv 2022年

作者： Samuel, Roshan Samtaney, Ravi Verma, Mahendra K. Department of Mechanical Engineering Indian Institute of Technology Kanpur208016 India Mechanical Engineering Program Physical Science and Engineering Division King Abdullah University of Science and Technology Thuwal 23955 Saudi Arabia Department of Physics Indian Institute of Technology Kanpur208016 India

We adopt the stretched spiral vortex sub-grid model for large-eddy simulation (LES) of turbulent convection at extreme Rayleigh numbers. We simulate Rayleigh-Bénard convection (RBC) for Rayleigh numbers ranging from 106 to 1015 and for Prandtl numbers 0.768 and 1. We choose a box of dimensions 1:1:10 to reduce computational cost. Our LES yields Nusselt and Reynolds numbers that are in good agreement with the direct-numerical simulation (DNS) results of Iyer et al.1, albeit with a smaller grid size and at significantly reduced computational expense. For example, in our simulations at Ra = 1013, we use grids that are 1/120 times the grid-resolution as that of the DNS1. The Reynolds numbers in our simulations span 3 orders of magnitude from 1,000 to 1,700,000. Consistent with the literature, we obtain scaling relations for Nusselt and Reynolds numbers as Nu ∼ Ra0.317 and Re ∼ Ra0.497. We also perform LES of RBC with periodic side-walls, for which we obtain the corresponding scaling exponents as 0.343 and 0.477 respectively. Our LES is a promising tool to push simulations of thermal convection to extreme Rayleigh numbers, and hence enable us to test the transition to ultimate convection regime. © 2022, CC BY.

关键词： Large eddy simulation

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Discovery of a Topological Charge Density Wave

arXiv

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arXiv 2024年

作者： Litskevich, Maksim Hossain, Shafayat Zhang, Songbo Cheng, Zi-Jia Guin, Satya N. Kumar, Nitesh Shekhar, Chandra Wang, Zhiwei Li, Yongkai Chang, Guoqing Yin, Jia-Xin Zhang, Qi Cheng, Guangming Jiang, Yu-Xiao Cochran, Tyler A. Shumiya, Nana Yang, Xian P. Multer, Daniel Liu, Xiaoxiong Yao, Nan Yao, Yugui Felser, Claudia Neupert, Titus Hasan, M. Zahid Department of Physics Princeton University PrincetonNJ United States Department of Physics University of Zurich Winterthurerstrasse Zurich Switzerland Max Planck Institute for Chemical Physics of Solids 16 Nöthnitzer Straße 40 Dresden01187 Germany School of Physics Beijing Institute of Technology Beijing100081 China Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing100190 China Division of Physics and Applied Physics School of Physical and Mathematical Sciences Nanyang Technological University Singapore Princeton Institute for Science and Technology of Materials Princeton University PrincetonNJ United States Lawrence Berkeley National Laboratory BerkeleyCA94720 United States

Charge density waves appear in numerous condensed matter platforms, ranging from high-temperature superconductors to quantum Hall systems. Despite such ubiquity, there has been a lack of direct experimental study on boundary states that can uniquely stem from the charge order. Here, using scanning tunneling microscopy, we directly visualize the bulk and boundary phenomenology of the charge density wave in a topological material, Ta2Se8I. Below the charge density wave transition temperature (TCDW 260 K), tunneling spectra on an atomically resolved lattice reveal a large insulating gap in the bulk and on the surface, exceeding 500 meV, surpassing predictions from standard weakly-coupled mean-field theory. Spectroscopic imaging confirms the presence of a charge density wave, with local density of states maxima at the conduction band corresponding to the local density of states minima at the valence band, thus revealing a π phase difference in the respective charge density wave order. Concomitantly, at a monolayer step edge, we detect an in-gap boundary mode (edge state) with modulations along the edge that match the charge density wave wavevector along the edge. Intriguingly, the phase of the edge state modulation shifts by π within the charge order gap, connecting the fully gapped bulk (and surface) conduction and valence bands via a smooth energy-phase relation. This bears similarity to the topological spectral flow of edge modes, where the boundary modes bridge the gapped bulk modes in energy and momentum magnitude but in Ta2Se8I, the connectivity distinctly occurs in energy and momentum phase. Notably, our temperature-dependent measurements indicate a vanishing of the insulating gap and the in-gap edge state above TCDW, suggesting their direct relation to the charge order. The theoretical analysis also indicates that the observed boundary mode is likely topological and linked to the charge order. Our study further illuminates a puzzle concerning the enigmatic groun

关键词： Topology

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Size-Dependent Redispersion or Agglomeration of Ag Clusters on CeO₂

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Journal of physical Chemistry C 2022年第28期126卷 11537-11543页

作者： Chang, Sujie Bao, Hongliang Huang, Weixin Hefei National Laboratory for Physical Sciences at the Microscale Key Lab. of Surf. and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes Department of Chemical Physics University of Science and Technology of China Hefei 230026 China School of Materials and Engineering Shandong Jianzhu University Jinan 250101 China Shanghai Institute of Applied Physics Chinese Academy of Sciences Shanghai 201800 China Dalian National Laboratory for Clean Energy Chinese Academy of Sciences Dalian 116023 China

Supported metal nanoparticles tend to agglomerate at high temperatures. Herein, we report that Ag clusters supported on CeO2 prepared by a deposition-precipitation method followed by calcination at 200 °C undergo size-dependent redispersion or agglomeration processes upon further calcination at 500 °C, accompanied by segregation and reduction of Ag+ cations dissolved in CeO2. Fine Ag clusters with a detectable Ag-O coordination shell using EXAFS redisperse, while large Ag clusters only with a detectable Ag-Ag coordination shell agglomerate. We propose that segregation and reduction of Ag+ cations dissolved in CeO2 upon calcination at 500 °C create additional surface oxygen vacancies capable of dismantling fine Ag clusters due to strong Ag-surface oxygen vacancy interaction. The catalytic activity of acquired Ag/CeO2 varies sensitively with the dispersions of supported Ag clusters. These results highlight the important role of surface restructuring of oxide supports in redispersing supported metal clusters. © 2022 American chemical Society.

关键词： Catalysts Extended X-ray absorption fine structure Metal clusters Redox reactions X-ray photoelectron spectroscopy

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Nanoslot-Induced Ultrastrong Phonon-Photon and Phonon-Phonon Coupling in Hybrid Organic-Inorganic Perovskites

Nanoslot-Induced Ultrastrong Phonon-Photon and Phonon-Phonon...

引用

Pacific Rim Conference on Lasers and Electro-Optics (CLEO/Pacific Rim)

作者： Dasom Kim Jin Hou Geon Lee Ayush Agrawal Sunghwan Kim Hao Zhang Di Bao Andrey Baydin Wenjing WU Fuyang Tay Shengxi Huang Daivd Hagenmüller Elbert E. M. Chia Dai-Sik Kim Minah Seo Aditya D. Mohite Junichiro Kono Applied Physics Graduate Program Smalley-Curl Institute Rice University Houston TX USA Department of Electrical and Computer Engineering Rice University Houston TX USA Department of Materials Science and NanoEngineering Rice University Houston TX USA Sensor System Research Center Korea Institute of Science and Technology Seoul Republic of Korea Department of Physics and Astronomy Seoul National University Seoul Republic of Korea Department of Chemical and Biomolecular Engineering Rice University Houston TX USA Department of Physics Long-wavelength Nanotechnology Laboratory Quantum Photonics Institute Ulsan National Institute of Science and Technology (UNIST) Ulsan Republic of Korea Division of Physics and Applied Physics School of Physical and Mathematical Sciences Nanyang Technological University Singapore Smalley-Curl institute Rice University Houston TX USA CESQ-ISIS (UMR 7006) Universite de Strasbourg and CNRS Strasbourg France KU-KIST Graduate School of Converging Science and Technology Korea University Seoul Republic of Korea Department of Physics and Astronomy Rice University Houston TX USA

Methods for harnessing vibrational states are desired for phonon-based technologies. We realized ultrastrong coupling of two phonon modes in perovskite materials induced by ultrastrong coupling with a common photonic ... 详细信息

ISBN: (数字)9798350372076

ISBN: (纸本)9798350372083

关键词： Couplings Phonons Laser modes Perovskites Electro-optical waveguides Photonics

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Cooperation and Competition in Synchronous Open Quantum Systems

arXiv

引用

arXiv 2023年

作者： Murtadho, Taufiq Vinjanampathy, Sai Thingna, Juzar Daejeon34126 Korea Republic of Basic Science Program Korea University of Science and Technology Daejeon34113 Korea Republic of School of Physical and Mathematical Science Nanyang Technological University Singapore639798 Singapore Department of Physics Indian Institute of Technology-Bombay Powai Mumbai400076 India Centre of Excellence in Quantum Information Computation Science and Technology Indian Institute of Technology Bombay Powai Mumbai400076 India Centre for Quantum Technologies National University of Singapore 3 Science Drive 2 Singapore117543 Singapore Department of Physics and Applied Physics University of Massachusetts LowellMA01854 United States

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. © 2023, CC BY.

关键词： Synchronization

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Multistate Control of Nonlinear Photocurrents in Optoferroelectrics via phase manipulation of light field

arXiv

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arXiv 2025年

作者： Kazempour, Ali Sisakht, Esmaeil Taghizadeh Okyay, Mahmut Sait Jiang, Xiao Sato, Shunsuke Park, Noejung Department of physics Payame Noor University PO BOX Tehran119395-3697 Iran Department of Physics Ulsan National Institute of Science and Technology Ulsan689-798 Korea Republic of Materials Science and Engineering Program Department of Chemical and Environmental Engineering University of California-Riverside RiversideCA92521 United States Center for Computational Sciences University of Tsukuba Tsukuba305-8577 Japan

Ultrafast optical control of ferroelectricity based on short and intense light can be utilized to achieve accurate manipulations of ferroelectric materials, which may pave a basis for future breakthrough in nonvolatile memories. Here, we demonstrate that phase manipulation of electric field in the strong field sub-cycle regime induces a nonlinear injection current, efficiently coupling with the topology of band structure and enabling dynamic reversal of both current and polarization. Our time-dependent first-principles calculations reveal that tuning the phase of linearly or circularly polarized light through time-varying chirp, or constant carrier envelop phases within sub-laser-cycle dynamics effectively breaks the time-reversal symmetry, allowing the control over current and electronic polarization reversal over multi-ferroelectric states. Our time- and momentum-resolved transverse current analysis reveal the significance of Berry curvature higher order poles in the apparent association between the odd (even) orders of Berry curvature multipoles to odd (even) pseudo-harmonics in driving polarization dynamics reversal. We suggest that these phase manipulations of short pulse waveform may lead to unprecedented accurate control of nonlinear photocurrents and polarization states, which facilitate the development of precise ultrafast opto-ferroelectric devices. © 2025, CC BY.

关键词： Ferroelectricity

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Synchronization Lower Bounds the Efficiency of Near-Degenerate Thermal Machines

arXiv

引用

arXiv 2023年

作者： Murtadho, Taufiq Thingna, Juzar Vinjanampathy, Sai Daejeon34126 Korea Republic of Basic Science Program Korea University of Science and Technology Daejeon34113 Korea Republic of School of Physical and Mathematical Science Nanyang Technological University Singapore639798 Singapore Department of Physics and Applied Physics University of Massachusetts LowellMA01854 United States Department of Physics Indian Institute of Technology-Bombay Powai Mumbai400076 India Centre of Excellence in Quantum Information Computation Science and Technology Indian Institute of Technology Bombay Powai Mumbai400076 India Centre for Quantum Technologies National University of Singapore 3 Science Drive 2 Singapore117543 Singapore

We study the relationship between quantum synchronization and the thermodynamic performance of a four-level near-degenerate extension of the Scovil–Schulz-DuBois thermal maser. We show how the existence of interacting coherences can potentially modify the relationship between synchronization and the coherent power output of such a maser. In particular, the cooperation and competition between interacting coherences, causes the coherent heat and efficiency to be bounded by the synchronization measure in addition to the well-studied power synchronization bound. Overall, our results highlight the role of quantum synchronization in the working of a thermal machine. © 2023, CC BY.

关键词： Synchronization

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Direct Visualization of a Disorder Driven Electronic Smectic Phase in Dirac Nodal Line Semimetal GdSbTe

arXiv

引用

arXiv 2024年

作者： Venkatesan, Balaji Guan, Syu-You Chang, Jen-Te Chiu, Shiang-Bin Yang, Po-Yuan Su, Chih-Chuan Chang, Tay-Rong Raju, Kalaivanan Sankar, Raman Fongchaiya, Somboon Chu, Ming-Wen Chang, Chia-Seng Chang, Guoqing Lin, Hsin Del Maestro, Adrian Kao, Ying-Jer Chuang, Tien-Ming Department of Physics National Taiwan University Taipei10617 Taiwan Nano Science and Technology Program Taiwan International Graduate Program Academia Sinica National Taiwan University Taipei11529 Taiwan Institute of Physics Academia Sinica Taipei11529 Taiwan Department of Physics National Cheng-Kung University Tainan701 Taiwan Center for Condensed Matter Sciences National Taiwan University Taipei10617 Taiwan Molecular Science and Technology Program Taiwan International Graduate Program Academia Sinica Taipei11529 Taiwan Division of Physics and Applied Physics School of Physical and Mathematical Sciences Nanyang Technological University 21 Nanyang Link 637371 Singapore Department of Physics and Astronomy University of Tennessee KnoxvilleTN37996 United States Institute for Advanced Materials & Manufacturing University of Tennessee KnoxvilleTN37996 United States Min H. Kao Department of Electrical Engineering and Computer Science University of Tennessee KnoxvilleTN37996 United States Center for Quantum Science and Technology National Taiwan University Taipei10607 Taiwan

Electronic liquid crystal (ELC) phases are spontaneous symmetry breaking states believed to arise from strong electron correlation in quantum materials such as cuprates and iron pnictides. Here, we report a direct observation of a smectic phase in a weakly correlated Dirac nodal line (DNL) semimetal GdSbxTe2-x. Incommensurate smectic charge modulation and intense local unidirectional nanostructure are visualized by using spectroscopic imaging - scanning tunneling microscopy. As topological materials with symmetry protected Dirac or Weyl fermions are mostly weakly correlated, the discovery of such an ELC phase are anomalous and raise questions on the origin of their emergence. Specifically, we demonstrate how chemical substitution generates these symmetry breaking phases before the system undergoes a charge density wave (CDW) - orthorhombic structural transition. Our results highlight the importance of impurities in realizing ELC phases and present a new material platform for exploring the interplay among quenched disorder, topology and electron correlation. Copyright © 2024, The Authors. All rights reserved.

关键词： Charge density waves

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Strong, Mid-IR Driven THz Generation for Nonlinear Spectroscopy

Strong, Mid-IR Driven THz Generation for Nonlinear Spectrosc...

引用

CLEO: science and Innovations in CLEO 2024, CLEO: S and I 2024 - Part of Conference on Lasers and Electro-Optics

作者： Gollner, Claudia Jutas, Rokas Kreil, Dominik Dirin, Dmitry N. Boehme, Simon C. Baltuška, Andrius Kovalenko, Maksym V. Koulouklidis, Anastasios D. Fedorov, Vladimir Yu. Tzortzakis, Stelios Shalaby, Mostafa Pugžlys, Audrius Stanford Institute for Materials & Energy Sciences SLAC National Accelerator Laboratory 2575 Sand Hill Rd Menlo ParkCA94025 United States Photonics Institute TU Wien Gusshausstrasse 27-387 WienA-1040 Austria Institute for Theoretical Physics Johannes Kepler University Altenbergerstraße 69 LinzA-4040 Austria Institute of Inorganic Chemistry Department of Chemistry and Applied Biosciences ETH Zürich 10 Vladimir Prelog Weg 1 ZürichCH-8093 Switzerland Empa-Swiss Federal Laboratories for Materials Science and Technology DübendorfCH-8600 Switzerland Center for Physical Sciences & Technology Savanoriu Ave. 231 VilniusLT-02300 Lithuania P.O. Box 1527 HeraklionGR-71110 Greece Science Program Texas A&M University at Qatar P.O. Box 23874 Doha Qatar P.N. Lebedev Physical Institute The Russian Academy of Sciences 53 Leninskiy Prospekt Moscow119991 Russia Department of Materials Science and Technology University of Crete HeraklionGR-71003 Greece Swiss Terahertz Research-Zurich Techpark Zurich8005 Switzerland Park Innovaare VilligenCH-5234 Switzerland Key Laboratory of Terahertz Optoelectronics Beijing Advnaced Innovation Center of Imaging Technology CNU Bejing100048 China

We report on strong-field THz sources from optical rectification in organic crystals or two-color plasma filaments, driven by intense mid-IR pulses. Non-linear perturbation of semiconductor materials is demonstrated b...

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