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SSRN 2024年

作者： Yusuf, Maha Kaestner, Anders Wied, Markus LaManna, Jacob M. Vo, Nghia T. Dunlop, Alison R. Jansen, Andrew N. Polzin, Bryant J. Trask, Stephen E. Strobl, Markus Wood, Vanessa Toney, Michael F. Weker, Johanna Nelson Department of Chemical Engineering StanfordCA94305 United States Laboratory for Neutron Scattering and Imaging Paul Scherrer Institut Forschungsstrasse 111 Villigen5232 Switzerland Department of Information Technology and Electrical Engineering ETH Zürich Gloriastrasse 35 Zürich8092 Switzerland National Institute of Standards and Technology GaithersburgMD20899 United States National Synchrotron Light Source II Brookhaven National Laboratory UptonNY11973-5000 United States Argonne National Laboratory 9700 South Cass Avenue LemontIL60439 United States Department of Chemical and Biological Engineering University of Colorado BoulderCO80309 United States Department of Materials science and Engineering University of Colorado BoulderCO80309 United States Renewable and Sustainable Energy Institute University of Colorado BoulderCO80309 United States Stanford Synchrotron Radiation Lightsource SLAC National Accelerator Laboratory Menlo ParkCA94025 United States

Mechanistic understanding of Li plating is imperative to developing fast-charging batteries for sustainable electric vehicles. Here, we report in-situ 3D characterization of the morphology and spatial heterogeneities of Li plating using neutron micro-computed tomography with a spatial resolution of 10-15 microns. Two batteries are imaged in charged and discharged states after: (1) 4 cycles of 1C and (2) 6 cycles of 6C charging. Neutron images show that Li plates at and around the edge of graphite, indicating that the graphite edge and the areas around the edge are the most susceptible to Li plating. However, certain areas of the cells form dead Li whereas others form active Li. We discuss the spatial heterogeneities in four regions: (1) near Cu current collector (CC), (2) in the middle of graphite electrode, (3) at the graphite-separator interface, and (4) in the separator. Specifically, Li near the Cu CC remains active, whereas Li near the interface and in the separator becomes dead at both 1C and 6C. Additionally, a distinct 3D Li morphology is revealed at 6C vs. 1C. Particularly, tip-like Li deposits are observed mostly at 6C that become dead following battery discharging, suggesting a correlation between higher XFC-charging rate/cycling number and the increased formation of tip-like dead Li deposits. © 2024, The Authors. All rights reserved.

关键词： Morphology

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Time Correlation Filtering Reveals Two-Path Electron Quantum Interference in Strong-Field Ionization

arXiv

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arXiv 2022年

作者： Werby, Nicholas Maxwell, Andrew S. Forbes, Ruaridh de Morisson Faria, Carla Figueira Bucksbaum, Philip H. Stanford PULSE Institute SLAC National Accelerator Laboratory 2575 Sand Hill Road Menlo ParkCA94025 United States Department of Physics Stanford University StanfordCA94305 United States Department of Physics and Astronomy Aarhus University Aarhus CDK-8000 Denmark Institut de Ciencies Fotoniques The Barcelona Institute of Science and Technology Castelldefels Barcelona08860 Spain Department of Physics & Astronomy University College London Gower Street LondonWC1E 6BT United Kingdom Linac Coherent Light Source SLAC National Accelerator Laboratory Menlo ParkCA94025 United States Department of Applied Physics Stanford University StanfordCA94305 United States

Attosecond dynamics in strong-field tunnel ionization are encoded in intricate holographic patterns in the photoelectron momentum distributions (PMDs). These patterns show the interference between two or more superposed quantum electron trajectories, which are defined by their ionization times and subsequent evolution in the laser field. We determine the ionization time separation between interfering pairs of electron orbits by performing a differential Fourier analysis on the measured momentum spectrum. We identify electron holograms formed by trajectory pairs whose ionization times are separated by less than a single quarter cycle, between a quarter cycle and half cycle, between a half cycle and three fourths of a cycle, and a full cycle apart. We compare our experimental results to the predictions of the Coulomb quantum orbit strong-field approximation (CQSFA), with significant success. We also time-filter the CQSFA trajectory calculations to demonstrate the validity of the technique on spectra with known time correlations. As a general analysis technique, the filter can be applied to all energy- and angularly-resolved datasets to recover time correlations between interfering electron pathways, providing an important tool to analyze any strong-field ionization spectra. © 2022, CC BY.

关键词： Electrons

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Observation of Flat Bands and Dirac Cones in a Pyrochlore Lattice Superconductor

arXiv

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arXiv 2023年

作者： Huang, Jianwei Setty, Chandan Deng, Liangzi You, Jing-Yang Liu, Hongxiong Shao, Sen Oh, Ji Seop Guo, Yucheng Zhang, Yichen Yue, Ziqin Yin, Jia-Xin Hashimoto, Makoto Lu, Donghui Gorovikov, Sergey Dai, Pengcheng Denlinger, Jonathan D. Hasan, M. Zahid Feng, Yuan-Ping Birgeneau, Robert J. Shi, Youguo Chu, Ching-Wu Chang, Guoqing Si, Qimiao Yi, Ming Department of Physics and Astronomy Rice Center for Quantum Materials Rice University HoustonTX77005 United States Department of Physics Texas Center for Superconductivity University of Houston HoustonTX77204 United States Department of Physics National University of Singapore 2 Science Drive 3 Singapore117551 Singapore 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 Singapore637371 Singapore Department of Physics University of California Berkeley BerkeleyCA94720 United States Department of Physics Princeton University PrincetonNJ08544 United States Stanford Synchrotron Radiation Lightsource SLAC National Accelerator Laboratory Menlo ParkCA94025 United States Canadian Light Source 44 Innovation Boulevard SaskatoonSKS7N 2V3 Canada Advanced Light Source Lawrence Berkeley National Laboratory BerkeleyCA94720 United States Princeton Institute for Science and Technology of Materials Princeton University PrincetonNJ08544 United States Centre for Advanced 2D Materials National University of Singapore 6 Science Drive 2 Singapore117546 Singapore Materials Sciences Division Lawrence Berkeley National Laboratory BerkeleyCA94720 United States Department of Materials Science and Engineering University of California BerkeleyCA94720 United States

Emergent phases often appear when the electronic kinetic energy is comparable to the Coulomb interactions. One approach to seek material systems as hosts of such emergent phases is to realize localization of electronic wavefunctions due to the geometric frustration inherent in the crystal structure, resulting in flat electronic bands. Recently, such efforts have found a wide range of exotic phases in the two-dimensional kagome lattice, including magnetic order, time-reversal symmetry breaking charge order, nematicity, and superconductivity. However, the interlayer coupling of the kagome layers disrupts the destructive interference needed to completely quench the kinetic energy. Here we demonstrate that an interwoven kagome network-a pyrochlore lattice-can host a three dimensional (3D) localization of electron wavefunctions. Meanwhile, the nonsymmorphic symmetry of the pyrochlore lattice guarantees all band crossings at the Brillouin zone X point to be 3D gapless Dirac points, which was predicted theoretically but never yet observed experimentally. Through a combination of angle-resolved photoemission spectroscopy, fundamental lattice model and density functional theory calculations, we investigate the novel electronic structure of a Laves phase superconductor with a pyrochlore sublattice, CeRu2. We observe flat bands originating from both the Ce 4f orbitals as well as from the 3D destructive interference of the Ru 4d orbitals. We further observe the nonsymmorphic symmetry-protected 3D gapless Dirac cones at the X point. Our work establishes the pyrochlore structure as a promising lattice platform to realize and tune novel emergent phases intertwining topology and many-body interactions. Copyright © 2023, The Authors. All rights reserved.

关键词： Superconducting materials

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Orbital-selective time-domain signature of nematicity dynamics in the charge-density-wave phase of La1.65Eu0.2Sr0.15CuO4

arXiv

引用

arXiv 2022年

作者： Bluschke, Martin Gupta, Naman K. Jang, Hoyoung Husain, Ali A. Lee, Byungjune Na, MengXing Remedios, Brandon Dos Smit, Steef Moen, Peter Park, Sang-Youn Kim, Minseok Jang, Dogeun Choi, Hyeongi Sutarto, Ronny Reid, Alexander H. Dakovski, Georgi L. Coslovich, Giacomo Nguyen, Quynh L. Burdet, Nicolas G. Lin, Ming-Fu Revcolevschi, Alexandre Park, Jae-Hoon Geck, Jochen Turner, Joshua J. Damascelli, Andrea Hawthorn, David G. Quantum Matter Institute University of British Columbia VancouverBCV6T 1Z4 Canada Department of Physics & Astronomy University of British Columbia VancouverBCV6T 1Z1 Canada Department of Physics & Astronomy University of Waterloo WaterlooONN2L 3G1 Canada PAL-XFEL Pohang Accelerator Laboratory Gyeongbuk Pohang37673 Korea Republic of Photon Science Center Pohang University of Science and Technology Gyeongbuk Pohang37673 Korea Republic of Max Planck POSTECH/Korea Research Initiative Center for Complex Phase Materials Pohang37673 Korea Republic of Department of Physics Pohang University of Science and Technology Pohang37673 Korea Republic of Canadian Light Source SaskatoonSKS7N 2V3 Canada Linac Coherent Light Source SLAC National Accelerator Laboratory Menlo ParkCA94025 United States Stanford PULSE Institute Stanford University SLAC National Accelerator Laboratory Menlo ParkCA94025 United States Stanford Institute for Materials and Energy Sciences SLAC National Accelerator Laboratory Stanford University Menlo ParkCA94025 United States Institut de Chimie Moléculaire et des Matériaux d’Orsay Université Paris-Saclay CNRS UMR 8182 Orsay91405 France Institute of Solid State and Materials Physics TU Dresden Dresden01069 Germany Würzburg-Dresden Cluster of Excellence ct.qmat Technische Universität Dresden Dresden01062 Germany

Understanding the interplay between charge, nematic, and structural ordering tendencies in cuprate superconductors is critical to unraveling their complex phase diagram. Using pump-probe time-resolved resonant x-ray scattering on the (0 0 1) Bragg peak at the Cu L3 and O K resonances, we investigate non-equilibrium dynamics of Qa = Qb = 0 nematic order and its association with both charge density wave (CDW) order and lattice dynamics in La1.65Eu0.2Sr0.15CuO4. The orbital selectivity of the resonant x-ray scattering cross-section allows nematicity dynamics associated with the planar O 2p and Cu 3d states to be distinguished from the response of anisotropic lattice distortions. A direct time-domain comparison of CDW translational-symmetry breaking and nematic rotational-symmetry breaking reveals that these broken symmetries remain closely linked in the photoexcited state, consistent with the stability of CDW topological defects in the investigated pump fluence regime. Copyright © 2022, The Authors. All rights reserved.

关键词： Charge density waves

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Electronic excitations of α−Fe2O3 heteroepitaxial films measured by resonant inelastic x-ray scattering at the Fe L edge

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Physical Review B 2022年第7期105卷 075101-075101页

作者： David S. Ellis Ru-Pan Wang Deniz Wong Jason K. Cooper Christian Schulz Yi-De Chuang Yifat Piekner Daniel A. Grave Markus Schleuning Dennis Friedrich Frank M. F. de Groot Avner Rothschild Department of Materials Science and Engineering Technion-Israel Institute of Technology Haifa 32000 Israel Department of Physics University of Hamburg Luruper Chaussee 149 22761 Hamburg Germany Dynamics and Transport in Quantum Materials Helmholtz-Zentrum Berlin für Materialen und Energie Albert-Einstein-Strasse 15 12489 Berlin Germany Chemical Sciences Division Lawrence Berkeley National Laboratory 1 Cyclotron Road Berkeley California 94720 USA Advanced Light Source Lawrence Berkeley National Laboratory 1 Cyclotron Road Berkeley California 94720 USA The Nancy & Stephen Grand Technion Energy Program (GTEP) Technion-Israel Institute of Technology Haifa 32000 Israel Department of Materials Engineering and Ilse Katz Institute for Nanoscale Science and Technology Ben Gurion University of the Negev Be'er Sheva 8410501 Israel Institute for Solar Fuels Helmholtz-Zentrum Berlin für Materialien und Energie GmbH Hahn-Meitner-Platz 1 14109 Berlin Germany Department of Inorganic Chemistry and Catalysis Debye Institute of Nanomaterials Science Utrecht University Universiteitsweg 99 3584 CG Utrecht Netherlands

Resonant inelastic x-ray scattering (RIXS) spectra of hematite (α−Fe2O3) were measured at the Fe L3 edge for heteroepitaxial thin films which were undoped and doped with 1% Ti, Sn, or Zn, in the energy-loss range in excess of 1 eV to study electronic transitions. The spectra were measured for several momentum transfers q, conducted at both low temperature (T=14 K) and room temperature. While we cannot rule out dispersive features possibly owing to propagating excitations, the coarse envelopes of the general spectra did not appreciably change shape with q, implying that the bulk of the observed L-edge RIXS intensity originates from (mostly) nondispersive ligand field excitations. Summing the RIXS spectra over q and comparing the results at T=14 K to those at T=300 K revealed pronounced temperature effects, including an intensity change and energy shift of the ≈1.4 eV peak, a broadband intensity increase of the 3–4 eV range, and higher energy features. The q-summed spectra and their temperature dependencies are virtually identical for nearly all of the samples with different dopants, save for the temperature dependence of the Ti-doped sample's spectrum, which we attribute to being affected by a large number of free charge carriers. Comparing with magnetization measurements for different temperatures and dopings likewise did not show a clear correlation between the RIXS spectra and the magnetic ordering states. To clarify the excited states, we performed spin multiplet calculations which were in excellent agreement with the RIXS spectra over a wide energy range and provide detailed electronic descriptions of the excited states. The implications of these findings to the photoconversion efficiency of hematite photoanodes is discussed.

关键词： Electronic structure Energy materials Strongly correlated systems Crystal-field theory Energy-dispersive x-ray spectroscopy

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Precise dd excitations and commensurate intersite Coulomb interactions in the dissimilar cuprate YBa2Cu3O7−y and La2-xSrxCuO4

arXiv

引用

arXiv 2023年

作者： Huang, Shih-Wen Wray, L. Andrew Shao, Yu-Cheng Wu, Cheng-Yau Wang, Shun-Hung Lee, Jenn-Min Chen, Y.-J. Schoenlein, R.W. Mou, C.Y. Chuang, Yi-De Lin, J.-Y. Swiss Light Source Paul Scherrer Institut Villigen PSICH5232 Switzerland MAX IV Laboratory Lund University P. O. Box 118 Lund221 00 Sweden Advanced Light Source Lawrence Berkeley National Laboratory BerkeleyCA94720 United States Materials Sciences Division Lawrence Berkeley National Laboratory BerkeleyCA94720 United States Department of Physics New York University New YorkNY10003 United States National Synchrotron Radiation Researc Center Hsinchu30076 Taiwan Institute of Physics National Yang Ming Chiao Tung University Hsinchu30010 Taiwan SLAC National Accelerator Laboratory Menlo ParkCA94025 United States Physics Division National Center for Theoretical Sciences P.O. Box 2-131 Hsinchu Taiwan Center for Quantum Technology Department of Physics National Tsing Hua University Hsinchu300 Taiwan Institute of Physics Academia Sinica Taipei11529 Taiwan Department of Physics National Tsing Hua University Hsinchu30043 Taiwan Center for Emergent Functional Matter Science National Yang Ming Chiao Tung University Hsinchu30010 Taiwan

Using high-resolution extreme ultraviolet resonant inelastic X-ray scattering (EUVRIXS) spectroscopy at Cu M-edge, we observed the doping dependent spectral shifts of inter-orbital (dd) excitations of YBa2Cu3O7−y and La2−xSrxCuO4. With increasing hole doping level from undoped to optimally doped superconducting compositions, the leading edge of dd excitations is found to shift towards lower energy loss in a roughly linear trend that is irrespective to the cuprate species. The magnitude of energy shift can be explained by including a 0.15 eV Coulomb attraction between Cu 3d(x2-y2) electrons and the doped holes on the surrounding oxygens in the atomic multiplet calculations. The consistent energy shift between distinct cuprate families suggests that this inter-site Coulomb interaction energy scale is relatively material-independent, and provides an important reference point for understanding charge density wave phenomena in the cuprate phase diagram. Copyright © 2023, The Authors. All rights reserved.

关键词： Copper compounds

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Universal orbital and magnetic structures in infinite-layer nickelates

arXiv

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arXiv 2023年

作者： Rossi, M. Lu, H. Lee, K. Goodge, B.H. Choi, J. Osada, M. Lee, Y. Li, D. Wang, B.Y. Jost, D. Agrestini, S. Garcia-Fernandez, M. Shen, Z.X. Zhou, Ke-Jin Been, E. Moritz, B. Kourkoutis, L.F. Devereaux, T.P. Hwang, H.Y. Lee, W.S. Stanford Institute for Materials and Energy Sciences SLAC National Accelerator Laboratory 2575 Sand Hill Road Menlo ParkCA94025 United States Department of Physics Stanford University StanfordCA94305 United States School of Applied and Engineering Physics Cornell University IthacaNY14850 United States Kavli Institute Cornell for Nanoscale Technology Cornell University IthacaNY14850 United States Diamond Light Source Harwell Campus DidcotOX11 0DE United Kingdom Department of Materials Science and Engineering Stanford University StanfordCA94305 United States Department of Applied Physics Stanford University StanfordCA94305 United States Geballe Laboratory for Advanced Materials Stanford University StanfordCA94305 United States

We conducted a comparative study of the rare-earth infinite-layer nickelates films, RNiO2 (R = La, Pr, and Nd) using resonant inelastic X-ray scattering (RIXS). We found that the gross features of the orbital configurations are essentially the same, with minor variations in the detailed hybridization. For low-energy excitations, we unambiguously confirm the presence of damped magnetic excitations in all three compounds. By fitting to a linear spin-wave theory, comparable spin exchange coupling strengths and damping coefficients are extracted, indicating a universal magnetic structure in the infinite-layer nickelates. Interestingly, while signatures of a charge order are observed in LaNiO2 in the quasi-elastic region of the RIXS spectrum, it is absent in NdNiO2 and PrNiO2. This prompts further investigation into the universality and the origins of charge order within the infinite-layer nickelates. Copyright © 2023, The Authors. All rights reserved.

关键词： Nickel compounds

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Structural properties of chalcogenide glasses and the isocoordination rule: Disentangling effects from chemistry and network topology

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Physical Review B 2022年第1期106卷 014206-014206页

作者： M. Micoulaut I. Pethes P. Jóvári L. Pusztai M. Krbal T. Wágner V. Prokop Š. Michalik K. Ikeda I. Kaban Sorbonne Université Laboratoire de Physique Théorique de la Matière Condensée CNRS UMR 7600 75252 Paris Cedex 05 France Institute for Solid State Physics and Optics Wigner Research Center H-1525 Budapest POB 49 Hungary IROAST Kumamoto University 2-39-1 Kurokami Chuo-ku Kumamoto 860-8555 Japan Center of Materials and Nanotechnologies Faculty of Chemical Technology University of Pardubice 6 Pardubice 53002 Czech Republic Department of General and Inorganic Chemistry Faculty of Chemical Technology University of Pardubice Pardubice 53210 Czech Republic Diamond Light Source Ltd. Harwell Science and Innovation Campus Didcot Oxfordshire OX11 0DE United Kindgom Institute of Materials Structure Science High Energy Accelerator Research Organization (KEK) Tokai Ibaraki 319-1106 Japan Leibniz-Institut für Festkörper- und Werkstoffforschung Dresden Institute for Complex Materials 01069 Dresden Germany

The structural properties of two Ge-As-Se glass compositions (Ge10As10Se80 and Ge21As21Se58) are investigated from a combination of density-functional-based molecular dynamics simulations and neutron/x-ray scattering experiments. We first focus on structural characteristics, including structure factors, pair distribution functions, angular distributions, coordination numbers, and neighbor distributions, and compare our results with the experimental data. Results leave anticipated coordinations from the octet rule (SeII, AsIII, and GeIV) unchanged, and these are contrasted with respect to glasses having the same average coordination number r¯ such as binary As30Se70 and Ge33Se67. The increase of (As,Ge) content induces a growth of ring structures that are dominated by edge-sharing motifs (four-membered rings) having mostly heteropolar bonds, while As-As and As-Ge homopolar bonds are clearly more favored than Ge-Ge. These features signal that both topological (rings) and chemical (bonds) features are different with respect to related binaries. The validity of the so-called vibrational isocoordination rule stating that properties of multicomponent chalcogenides depend solely on r¯ is checked, and results from a vibrational analysis indicates that this rule is merely satisfied for the Se-rich composition. An inspection of correlations via the Bhatia-Thornton formalism shows that topological ordering is not only different between Ge10As10Se80 and Ge21As21Se58 but also radically contrasts with respect to the isocoordinated binary glasses and displays an obvious reduced directional bonding.

关键词： Network structure Glasses Molecular dynamics Neutron scattering X-ray scattering

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Topology hierarchy of transition metal dichalcogenides built from quantum spin Hall layers

arXiv

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arXiv 2023年

作者： Xu, Lixuan Li, Yiwei Fang, Yuqiang Zheng, Huijun Shi, Wujun Chen, Cheng Pei, Ding Lu, Donghui Hashimoto, Makoto Wang, Meixiao Yang, Lexian Feng, Xiao Zhang, Haijun Huang, Fuqiang Xue, Qikun He, Ke Liu, Zhongkai Chen, Yulin State Key Laboratory of Low Dimensional Quantum Physics Department of Physics Tsinghua University Beijing100084 China Wuhan University Wuhan430072 China School of Physical Science and Technology ShanghaiTech University Shanghai201210 China State Key Laboratory of Rare Earth Materials Chemistry and Applications College of Chemistry and Molecular Engineering Peking University Beijing100871 China ShanghaiTech Laboratory for Topological Physics Shanghai201210 China Center for Transformative Science ShanghaiTech University Shanghai201210 China ShanghaiTech University Shanghai201210 China Advanced Light Source Lawrence Berkeley National Laboratory BerkeleyCA94720 United States Stanford Synchrotron Radiation Lightsource SLAC National Accelerator Laboratory Menlo ParkCA94025 United States National Laboratory of Solid State Microstructures School of Physics Nanjing University Nanjing210093 China Clarendon LaboratoryDepartment of Physics University of Oxford OxfordOX1 3PU United Kingdom

The evolution of the physical properties of two-dimensional material from monolayer limit to the bulk reveals unique consequences from dimension confinement and provides a distinct tuning knob for applications. Monolayer 1T’-phase transition metal dichalcogenides (1T’-TMDs) with ubiquitous quantum spin Hall (QSH) states are ideal two-dimensional building blocks of various three-dimensional topological phases. However, the stacking geometry was previously limited to the bulk 1T’-WTe2 type. Here, we introduce the novel 2M-TMDs consisting of translationally stacked 1T’-monolayers as promising material platforms with tunable inverted bandgaps and interlayer coupling. By performing advanced polarization-dependent angle-resolved photoemission spectroscopy as well as first-principles calculations on the electronic structure of 2M-TMDs, we revealed a topology hierarchy: 2M-WSe2, MoS2, and MoSe2 are weak topological insulators (WTIs), whereas 2M-WS2 is a strong topological insulator (STI). Further demonstration of topological phase transitions by tunning interlayer distance indicates that band inversion amplitude and interlayer coupling jointly determine different topological states in 2M-TMDs. We propose that 2M-TMDs are parent compounds of various exotic phases including topological superconductors and promise great application potentials in quantum electronics due to their flexibility in patterning with two-dimensional materials. © 2023, CC BY-NC-ND.

关键词： Topology

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In situ coherent x-ray scattering reveals polycrystalline structure and discrete annealing events in strongly coupled nanocrystal superlattices

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Physical Review Research 2024年第2期6卷 023119-023119页

作者： Matthew J. Hurley Christian P. N. Tanner Joshua Portner James K. Utterback Igor Coropceanu Avishek Das Joseph D. Slivka Andrei Fluerasu Yanwen Sun Sanghoon Song Leo M. Hamerlynck Alexander H. Miller Priyadarshini Bhattacharyya Dmitri V. Talapin Garth J. Williams Naomi S. Ginsberg Samuel W. Teitelbaum Department of Physics Arizona State University Tempe Arizona 85287 USA Department of Chemistry University of California Berkeley California 94720 USA Department of Chemistry James Franck Institute and Pritzker School of Molecular Engineering University of Chicago Chicago Illinois 60637 USA Department of Physics University of California Berkeley California 94720 USA Brookhaven National Laboratory NSLS-II Upton New York 11973 USA Linac Coherent Light Source SLAC National Accelerator Laboratory Menlo Park California 94025 USA School for Engineering of Matter Transport and Energy Arizona State University Tempe Arizona 85287 USA Center for Nanoscale Materials Argonne National Laboratory Argonne Illinois 60517 USA Molecular Biophysics and Integrated Bioimaging Division Lawrence Berkeley National Laboratory Berkeley California 94720 USA Materials Sciences and Chemical Sciences Division Lawrence Berkeley National Laboratory Berkeley California 94720 USA Kavli Energy NanoSciences Institute University of California Berkeley California 94720 USA STROBE NSF Science & Technology Center Berkeley California 94720 USA

Solution-phase bottom up self-assembly of nanocrystals into superstructures such as ordered superlattices is an attractive strategy to generate functional materials of increasing complexity, including very recent advances that incorporate strong interparticle electronic coupling. While the self-assembly kinetics in these systems have been elucidated and related to the product characteristics, the weak interparticle bonding interactions suggest the superstructures formed could continue to order within the solution long after the primary nucleation and growth have occurred, even though the mechanism of annealing remains to be elucidated. Here, we use a combination of Bragg coherent diffractive imaging and x-ray photon correlation spectroscopy to create real-space maps of supercrystalline order along with a real-time view of the strain fluctuations in aging strongly coupled nanocrystal superlattices while they remain suspended and immobilized in solution. By combining the results, we deduce that the self-assembled superstructures are polycrystalline, initially comprising multiple nucleation sites, and that shear avalanches at grain boundaries continue to increase crystallinity long after growth has substantially slowed. This multimodal approach should be generalizable to characterize a breadth of materials in situ in their native chemical environments, thus extending the reach of high-resolution coherent x-ray characterization to the benefit of a much wider range of physical systems.

关键词： Aging Defects Functional materials Self-assembly Heterostructures Nanoparticles Superlattices Coherent X-ray scattering X-ray photon correlation spectroscopy X-ray scattering

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