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Nature communications 2025年第1期16卷 863页

作者： Hao Chen Zan Lian Xiao Zhao Jiawei Wan Priscilla F Pieters Judit Oliver-Meseguer Ji Yang Elzbieta Pach Sophie Carenco Laureline Treps Nikos Liakakos Yu Shan Virginia Altoe Ed Wong Zengqing Zhuo Feipeng Yang Ji Su Jinghua Guo Monika Blum Saul H Lapidus Adrian Hunt Iradwikanari Waluyo Hirohito Ogasawara Haimei Zheng Peidong Yang Alexis T Bell Núria López Miquel Salmeron Chemical Sciences Division Lawrence Berkeley National Laboratory Berkeley CA USA. Institute of Chemical Research of Catalonia (ICIQ-CERCA) Barcelona Institute of Science and Technology (BIST) Tarragona Spain. Materials Science Division Lawrence Berkeley National Laboratory Berkeley CA USA. Department of Materials Science and Engineering University of California Berkeley CA USA. Department of Chemistry University of California Berkeley CA USA. Molecular Foundry Lawrence Berkeley National Laboratory Berkeley CA USA. Advanced Light Source Lawrence Berkeley National Laboratory Berkeley CA USA. Advanced Photon Source Argonne National Laboratory Lemont IL USA. National Synchrotron Light Source II Brookhaven National Laboratory Upton NY USA. SLAC National Accelerator Laboratory Menlo Park CA USA. Department of Chemical and Biomolecular Engineering University of California Berkeley CA USA. Chemical Sciences Division Lawrence Berkeley National Laboratory Berkeley CA USA. mbsalmeron@lbl.gov. Materials Science Division Lawrence Berkeley National Laboratory Berkeley CA USA. mbsalmeron@lbl.gov. Department of Materials Science and Engineering University of California Berkeley CA USA. mbsalmeron@lbl.gov.

Toughening mechanisms of the elytra of the diabolical ironclad beetle (vol 586, pg 543, 2020)

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NATURE 2021年第7844期590卷 E21-E21页

作者： Rivera, Jesus Hosseini, Maryam Sadat Restrepo, David Murata, Satoshi Vasile, Drago Parkinson, Dilworth Y. Barnard, Harold S. Arakaki, Atsushi Zavattieri, Pablo Kisailus, David Materials Science and Engineering Program University of California Riverside CA USA Department of Chemical and Environmental Engineering University of California Riverside CA USA Department of Materials Science and Engineering University of California Irvine CA USA Lyles School of Civil Engineering Purdue University West Lafayette IN USA Department of Mechanical Engineering The University of Texas at San Antonio San Antonio TX USA Institute of Global Innovation Research Tokyo University of Agriculture and Technology Koganei Tokyo Japan Advanced Light Source Lawrence Berkeley National Laboratory Berkeley CA USA

Unraveling iron oxides as abiotic catalysts of organic phosphorus recycling in soil and sediment matrices (vol 15, 5930, 2024)

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NATURE COMMUNICATIONS 2024年第1期15卷 5930页

作者： Basinski, Jade J. Bone, Sharon E. Klein, Annaleise R. Thongsomboon, Wiriya Mitchell, Valerie Shukle, John T. Druschel, Gregory K. Thompson, Aaron Aristilde, Ludmilla Northwestern University Department of Civil and Environmental Engineering Evanston USA (GRID:grid.16753.36) (ISNI:0000 0001 2299 3507) SLAC National Accelerator Laboratory Stanford Synchrotron Radiation Light Source Menlo Park USA (GRID:grid.445003.6) (ISNI:0000 0001 0725 7771) Northwestern University Department of Civil and Environmental Engineering Evanston USA (GRID:grid.16753.36) (ISNI:0000 0001 2299 3507) Australian Nuclear Science and Technology Organisation Australian Synchrotron Clayton Australia (GRID:grid.1089.0) (ISNI:0000 0004 0432 8812) Northwestern University Department of Civil and Environmental Engineering Evanston USA (GRID:grid.16753.36) (ISNI:0000 0001 2299 3507) Mahasarakham University Department of Chemistry Mahasarakham Thailand (GRID:grid.411538.a) (ISNI:0000 0001 1887 7220) Australian Nuclear Science and Technology Organisation Australian Synchrotron Clayton Australia (GRID:grid.1089.0) (ISNI:0000 0004 0432 8812) Indiana University-Purdue University Indianapolis Department of Earth Sciences Indianapolis USA (GRID:grid.257413.6) (ISNI:0000 0001 2287 3919) ZevRoss Spatial Analysis Ithaca USA (GRID:grid.257413.6) Indiana University-Purdue University Indianapolis Department of Earth Sciences Indianapolis USA (GRID:grid.257413.6) (ISNI:0000 0001 2287 3919) University of Georgia Department of Crop and Soil Sciences Athens USA (GRID:grid.213876.9) (ISNI:0000 0004 1936 738X)

In biogeochemical phosphorus cycling, iron oxide minerals are acknowledged as strong adsorbents of inorganic and organic phosphorus. Dephosphorylation of organic phosphorus is attributed only to biological processes, but iron oxides could also catalyze this reaction. Evidence of this abiotic catalysis has relied on monitoring products in solution, thereby ignoring iron oxides as both catalysts and adsorbents. Here we apply high-resolution mass spectrometry and X-ray absorption spectroscopy to characterize dissolved and particulate phosphorus species, respectively. In soil and sediment samples reacted with ribonucleotides, we uncover the abiotic production of particulate inorganic phosphate associated specifically with iron oxides. Reactions of various organic phosphorus compounds with the different minerals identified in the environmental samples reveal up to twenty-fold greater catalytic reactivities with iron oxides than with silicate and aluminosilicate minerals. Importantly, accounting for inorganic phosphate both in solution and mineral-bound, the dephosphorylation rates of iron oxides were within reported enzymatic rates in soils. Our findings thus imply a missing abiotic axiom for organic phosphorus mineralization in phosphorus *** oxides serve as both adsorbents and catalysts to generate inorganic phosphorus from organic phosphorus in environmental matrices. This abiotic dephosphorylation, which is comparable to enzymatic rates, is a missing piece in phosphorus cycling.

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Direct momentum imaging of charge transfer following site-selective ionization

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Physical Review A 2023年第4期108卷 043113-043113页

作者： Felix Allum Yoshiaki Kumagai Kiyonobu Nagaya James Harries Hiroshi Iwayama Mathew Britton Philip H. Bucksbaum Michael Burt Mark Brouard Briony Downes-Ward Taran Driver David Heathcote Paul Hockett Andrew J. Howard Jason W. L. Lee Yusong Liu Edwin Kukk Joseph W. McManus Dennis Milsesevic Akinobu Niozu Johannes Niskanen Andrew J. Orr-Ewing Shigeki Owada Patrick A. Robertson Artem Rudenko Kiyoshi Ueda James Unwin Claire Vallance Tiffany Walmsley Russell S. Minns Daniel Rolles Michael N. R. Ashfold Ruaridh Forbes Chemistry Research Laboratory Department of Chemistry University of Oxford Oxford OX1 3TA UK PULSE Institute SLAC National Accelerator Laboratory 2575 Sand Hill Road Menlo Park California 94025 USA Linac Coherent Light Source SLAC National Accelerator Laboratory 2575 Sand Hill Road Menlo Park California 94025 USA Department of Applied Physics Tokyo University of Agriculture and Technology Tokyo Japan Department of Physics Kyoto University Kyoto 606-8502 Japan QST SPring-8 Kouto 1-1-1 Sayo Hyogo Japan Institute for Molecular Science Okazaki 444-8585 Japan Sokendai (The Graduate University for Advanced Studies) Okazaki 444-8585 Japan School of Chemistry University of Southampton Highfield Southampton SO17 1BJ UK National Research Council of Canada 100 Sussex Dr. Ottawa ON K1A 0R6 Canada Deutsches Elektronen-Synchrotron DESY Hamburg Germany Department of Physics and Astronomy University of Turku FI-20014 Turku Finland Graduate School of Advanced Science and Engineering Hiroshima University Higashi-Hiroshima 739-8526 Japan School of Chemistry University of Bristol Cantock's Close Bristol BS8 1TS UK RIKEN SPring-8 Center Sayo Hyogo 679-5148 Japan Japan Synchrotron Radiation Research Institute Sayo Hyogo 679-5198 Japan J.R. Macdonald Laboratory Department of Physics Kansas State University Manhattan Kansas 66506 USA Department of Chemistry Tohoku University Sendai 980-8578 Japan

We study ultrafast charge rearrangement in dissociating 2-iodopropane (2−C3H7I) using site-selective core ionization at the iodine atom. Clear signatures of electron transfer between the neutral propyl fragment and multiply charged iodine ions are observed in the recorded delay-dependent ion momentum distributions. The detected charge-transfer pathway is only favorable within a small (few angstroms), charge-state-dependent spatial window located at C-I distances longer than that of the neutral ground-state molecule. These results offer insights into the physics underpinning charge transfer in isolated molecules and pave the way for a different class of time-resolved studies.

关键词： Autoionization & Auger processes Electronic excitation & ionization Electronic structure of atoms & molecules Multiphoton or tunneling ionization & excitation Photoemission Single- and few-photon ionization & excitation Ultrafast phenomena

Nanoscale visualization and spectral fingerprints of the charge order in ScV6Sn6 distinct from other kagome metals

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arXiv 2023年

作者： Cheng, Siyu Ren, Zheng Li, Hong Oh, Ji Seop Tan, Hengxin Pokharel, Ganesh DeStefano, Jonathan M. Rosenberg, Elliott Guo, Yucheng Zhang, Yichen Yue, Ziqin Lee, Yongbin Gorovikov, Sergey Zonno, Marta Hashimoto, Makoto Lu, Donghui Ke, Liqin Mazzola, Federico Kono, Junichiro Birgeneau, R.J. Chu, Jiun-Haw Wilson, Stephen D. Wang, Ziqiang Yan, Binghai Yi, Ming Zeljkovic, Ilija Department of Physics Boston College Chestnut HillMA02467 United States Department of Physics and Astronomy Rice University HoustonTX77005 United States Department of Physics University of California BerkeleyCA94720 United States Department of Condensed Matter Physics Weizmann Institute of Science Rehovot Israel Materials Department University of California Santa Barbara Santa BarbaraCA93106 United States Department of Physics University of Washington SeattleWA98195 United States Ames Laboratory AmesIA50011 United States Canadian Light Source Inc. 44 Innovation Boulevard SaskatoonSKS7N 2V3 Canada Stanford Synchrotron Radiation Lightsource SLAC National Accelerator Laboratory Menlo ParkCA94025 United States CNR Laboratorio TASC Area Science Park S.S.14 km 163.5 TriesteI-34149 Italy Department of Molecular Sciences and Nanosystems Ca' Foscari University of Venice Venice30172 Italy Materials Science Division Lawrence Berkeley National Laboratory BerkeleyCA94720 United States Applied Physics Graduate Program Smalley‐Curl Institute Rice University HoustonTX77005 United States

Charge density waves (CDWs) have been tied to a number of unusual phenomena in kagome metals, including rotation symmetry breaking, time‐reversal symmetry breaking and superconductivity. The majority of the experiments in kagome metals thus far have focused on the CDW states in AV3Sb5 (A=K, Cs, Rb) and FeGe, characterized by the 2a0 by 2a0 CDW period in the kagome plane. Recently, a bulk CDW phase (TCDW ≈ 92 K) with an entirely different wave length and orientation has been reported in ScV6Sn6, as the first realization of a CDW state in the broad RM6X6 crystal structure. Here, using a combination of scanning tunneling microscopy/spectroscopy and angle‐resolved photoemission spectroscopy, we reveal the microscopic structure and the spectroscopic signatures of this charge ordering phase in ScV6Sn6. Differential conductance dI/dV spectra show a partial gap opening in the density‐of‐states of about 20 meV at the Fermi level. This is much smaller than the spectral gaps observed in AV3Sb5 and FeGe despite the comparable TCDW temperatures in these systems, suggesting substantially weaker coupling strength in ScV6Sn6. Surprisingly, despite the three‐dimensional bulk nature of the charge order, we find that the charge modulation is only observed on the kagome termination. Temperature‐dependent band structure evolution suggests a modulation of the surface states as a consequence of the emergent charge order, with an abrupt spectral weight shift below TCDW consistent with the first‐order phase transition. The similarity of the electronic band structures of ScV6Sn6 and TbV6Sn6 (where the charge ordering is absent), together with the first‐principle calculations, suggests that charge ordering in ScV6Sn6 may not be primarily electronically driven. Interestingly, in sharp contrast to the CDW state of cousin AV3Sb5, we find no evidence supporting rotation symmetry breaking. Our results reveal a distinctive nature of the charge ordering phase in ScV6Sn6 in comparison to other kagome

关键词： Charge density waves

Real-space observation of the dissociation of a transition metal complex and its concurrent energy redistribution

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Nature Communications 2025年第1期16卷 1-9页

作者： Schori, Aviad Biasin, Elisa Banerjee, Ambar Boutet, Sébastien Bucksbaum, Philip H. Carbajo, Sergio Gaffney, Kelly J. Glownia, James M. Hartsock, Robert Ledbetter, Kathryn Kaldun, Andreas Koglin, Jason E. Kunnus, Kristjan Lane, Thomas J. Liang, Mengning Minitti, Michael P. O’Neal, Jordan T. Parrish, Robert M. Poitevin, Frédéric Ruddock, Jennifer M. Nelson, Silke Stankus, Brian Weber, Peter M. Wolf, Thomas J. A. Odelius, Michael Natan, Adi Stanford PULSE Institute SLAC National Accelerator Laboratory Menlo Park CA United States Physical Sciences Division Pacific Northwest National Laboratory Richland WA United States Department of Physics Stockholm University Stockholm Sweden Research Institute for Sustainable Energy (RISE) TCG Centres for Research and Education in Science and Technology Kolkata India Linac Coherent Light Source SLAC National Accelerator Laboratory Menlo Park CA United States Department of Physics Stanford University Stanford CA United States Department of Chemistry Stanford University Stanford CA United States Department of Chemistry Brown University Providence RI United States Department of Chemistry and Biochemistry Western Connecticut State University Danbury CT United States

Mechanistic insights into photodissociation dynamics of transition metal carbonyls, like Fe(CO)5, are fundamental for understanding active catalytic intermediates. Although extensively studied, the structural dynamics of these systems remain elusive. Using ultrafast X-ray scattering, we uncover the photochemistry of Fe(CO)5 in real space and time, observing synchronous oscillations in atomic pair distances, followed by a prompt rotating CO release preferentially in the axial direction. This behavior aligns with simulations, reflecting the interplay between the axial Fe-C distances’ potential energy landscape and non-adiabatic transitions between metal-to-ligand charge-transfer states. Additionally, we characterize a secondary delayed CO release associated with a reduction of Fe-C steady state distances and structural dynamics of the formed Fe(CO)4. Our results quantify energy redistribution across vibration, rotation, and translation degrees of freedom, offering a microscopic view of complex structural dynamics, enhancing our grasp on Fe(CO)5 photodissociation, and advancing our understanding of transition metal catalytic systems. © The Author(s) 2025.

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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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arXiv 2024年

作者： Hurley, Matthew J. Tanner, Christian P.N. Portner, Joshua Utterback, James K. Coropceanu, Igor Williams, Garth J. Das, Avishek Fluerasu, Andrei Sun, Yanwen Song, Sanghoon Hamerlynck, Leo M. Miller, Alexander H. Bhattacharyya, Priyadarshini Talapin, Dmitri V. Ginsberg, Naomi S. Teitelbaum, Samuel W. Department of Physics Arizona State University TempeAZ85287 United States Department of Chemistry University of California BerkeleyCA94720 United States Department of Chemistry James Franck Institute Pritzker School of Molecular Engineering University of Chicago ChicagoIL60637 United States Brookhaven National Laboratory NSLS-II UptonNY11973 United States Linac Coherent Light Source SLAC National Accelerator Laboratory Menlo ParkCA94025 United States School for Engineering of Matter Transport and Energy Arizona State University TempeAZ85287 United States Center for Nanoscale Materials Argonne National Laboratory ArgonneIL60517 United States Department of Physics University of California BerkeleyCA94720 United States Molecular Biophysics and Integrated Bioimaging Division Lawrence Berkeley National Laboratory BerkeleyCA94720 United States Materials Sciences and Chemical Sciences Division Lawrence Berkeley National Laboratory BerkeleyCA94720 United States Kavli Energy NanoSciences Institute University of California BerkeleyCA94720 United States STROBE NSF Science & Technology Center BerkeleyCA94720 United States

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. Copyright © 2024, The Authors. All rights reserved.

关键词： Nanocrystals

Kondo interaction in FeTe and its potential role in the magnetic order

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arXiv 2022年

作者： Kim, Younsik Kim, Minsoo Kim, Min-Seok Cheng, Cheng-Maw Choi, Joonyoung Jung, Saegyeol Lu, Donghui Kim, Jong Hyuk Cho, Soohyun Song, Dongjoon Oh, Dongjin Yu, Li Choi, Young Jai Kim, Hyeong-Do Han, Jung Hoon Jo, Younjung Seo, Jungpil Huh, Soonsang Kim, Changyoung Center for Correlated Electron Systems Institute for Basic Science Seoul08826 Korea Republic of Department of Physics & Astronomy Seoul National University Seoul08826 Korea Republic of Department of Emerging Materials Science DGIST Daegu42988 Korea Republic of National Synchrotron Radiation Research Center Hsinchu300 Taiwan Department of Physics Kyungpook National University Daegu38869 Korea Republic of Stanford Synchrotron Radiation Light source SLAC National Accelerator Laboratory CA94025 United States Department of Physics Yonsei University Seoul03021 Korea Republic of Center for Excellence in Superconducting Electronics State Key Laboratory of Functional Materials for Informatics Shanghai Institute of Microsystem and Information Technology Chinese Academy of Sciences Shanghai200050 China Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing100190 China School of Physical Sciences University of Chinese Academy of Sciences Beijing100049 China Songshan Lake Materials Laboratory Guangdong Dongguan523808 China XFEL Beamline Division Pohang Accelerator Laboratory Pohang37673 Korea Republic of Department of Physics Sungkyunkwan University Suwon16419 Korea Republic of

Finding d-electron heavy fermion (HF) states has been an important topic as the diversity in d-electron materials can lead to many exotic Kondo effect-related phenomena or new states of matter such as correlation-driven topological Kondo insulator or cooperation between long-range magnetism and Kondo lattice behavior. Yet, obtaining direct spectroscopic evidence for a d-electron HF system has been elusive to date. Here, we report the observation of Kondo lattice behavior in an antiferromagnetic metal, FeTe, via angle-resolved photoemission spectroscopy (ARPES) and transport properties measurements. The Kondo lattice behavior is represented by the emergence of a sharp quasiparticle at low temperatures. The transport property measurements confirm the low-temperature Fermi liquid behavior and reveal successive coherent-incoherent crossover upon increasing temperature. We interpret the Kondo lattice behavior as a result of hybridization between localized Fe 3dxy and itinerant Te 5pz orbitals. Our interpretation is further evidenced by Fano-type tunneling spectra which accompany a hybridization gap. Our observations strongly suggest unusual cooperation between Kondo lattice behavior and long-range magnetic order. © 2022, CC BY.

关键词： Transport properties

Evidence for a spinon Kondo effect in cobalt atoms on single-layer 1T-TaSe2

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arXiv 2022年

作者： Chen, Yi He, Wen-Yu Ruan, Wei Hwang, Jinwoong Tang, Shujie Lee, Ryan L. Wu, Meng Zhu, Tiancong Zhang, Canxun Ryu, Hyejin Wang, Feng Louie, Steven G. Shen, Zhi-Xun Mo, Sung-Kwan Lee, Patrick A. Crommie, Michael F. Department of Physics University of California BerkeleyCA94720 United States Materials Sciences Division Lawrence Berkeley National Laboratory BerkeleyCA94720 United States Department of Physics Massachusetts Institute of Technology CambridgeMA02139 United States Department of Physics Fudan University Shanghai200438 China Advanced Light Source Lawrence Berkeley National Laboratory BerkeleyCA94720 United States Stanford Institute for Materials and Energy Sciences SLAC National Accelerator Laboratory Stanford University Menlo ParkCA94025 United States Department of Physics Pusan National University Busan46241 Korea Republic of Geballe Laboratory for Advanced Materials Departments of Physics and Applied Physics Stanford University StanfordCA94305 United States CAS Center for Excellence in Superconducting Electronics Shanghai Institute of Microsystem and Information Technology Chinese Academy of Sciences Shanghai200050 China School of Physical Science and Technology Shanghai Tech University Shanghai200031 China Kavli Energy Nano Sciences Institute University of California Berkeley Lawrence Berkeley National Laboratory BerkeleyCA94720 United States Center for Spintronics Korea Institute of Science and Technology Seoul02792 Korea Republic of

Quantum spin liquids (QSLs) are highly entangled, disordered magnetic states that arise in frustrated Mott insulators and host exotic fractional excitations such as spinons and chargons. Despite being charge insulators some QSLs are predicted to exhibit gapless itinerant spinons that yield metallic behavior in the spin channel. We have deposited isolated magnetic atoms onto single-layer (SL) 1T-TaSe2, a gapless QSL candidate, to experimentally probe how itinerant spinons couple to impurity spin centers. Using scanning tunneling spectroscopy we observe the emergence of new, impurity-induced resonance peaks at the 1T-TaSe2 Hubbard band edges when cobalt adatoms are positioned to have maximal spatial overlap with the Hubbard band charge distribution. These resonance peaks disappear when the spatial overlap is reduced or when the magnetic impurities are replaced with non-magnetic impurities. Theoretical simulations using a modified Anderson impurity model integrated with a gapless quantum spin liquid show that these resonance peaks are consistent with a Kondo resonance induced by spinons combined with spinon-chargon binding effects that arise due to QSL gauge-field fluctuations. Copyright © 2022, The Authors. All rights reserved.

关键词： Cobalt

Enhancing nanoscale charged colloid crystallization near a metastable liquid binodal

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arXiv 2024年

作者： Tanner, Christian P.N. Wall, Vivian R.K. Portner, Joshua Jeong, Ahhyun Das, Avishek Utterback, James K. Hamerlynck, Leo M. Raybin, Jonathan G. Hurley, Matthew J. Leonard, Nicholas Wai, Rebecca B. Tan, Jenna A. Gababa, Mumtaz Zhu, Chenhui Schaible, Eric Tassone, Christopher J. Limmer, David T. Teitelbaum, Samuel W. Talapin, Dmitri V. Ginsberg, Naomi S. Department of Chemistry University of California BerkeleyCA94720 United States Department of Chemistry James Franck Institute Pritzker School of Molecular Engineering University of Chicago ChicagoIL60637 United States Department of Physics Arizona State University TempeAZ85287 United States Advanced Light Source Lawrence Berkeley National Laboratory BerkeleyCA94720 United States Stanford Synchrotron Radiation Lightsource SLAC National Accelerator Laboratory Menlo ParkCA94025 United States Chemical Sciences and Materials Sciences Divisions Lawrence Berkeley National Laboratory BerkeleyCA94720 United States Kavli Energy NanoSciences Institute University of California BerkeleyCA94720 United States Center for Nanoscale Materials Argonne National Laboratory ArgonneIL60517 United States Department of Physics University of California BerkeleyCA94720 United States Molecular Biophysics and Integrated Bioimaging Division Lawrence Berkeley National Laboratory BerkeleyCA94720 United States Materials Sciences and Chemical Sciences Division Lawrence Berkeley National Laboratory BerkeleyCA94720 United States STROBE NSF Science & Technology Center BerkeleyCA94720 United States

Achieving predictive control over crystallization using non-classical nucleation while avoiding kinetic traps is a roadblock toward designing materials with new functionalities. We address these challenges by inducing bottom-up assembly of nanocrystals (NCs) into ordered arrays, or superlattices (SLs). Using electrostatics, rather than density, to tune the interactions between particles, we watch self-assembly proceeding through a metastable liquid phase. We systematically investigate the phase behavior as a function of quench conditions in situ and in real time using small angle X-ray scattering (SAXS). Through quantitative fitting to colloid, liquid, and SL models, we extract the time evolution of each phase and the system phase diagram, which we find to be consistent with short-range attractive interactions. Using the phase diagram’s predictive power, we establish control of the self-assembly rate over three orders of magnitude, and identify one- and two-step self-assembly regimes, with only the latter implicating the metastable liquid as an intermediate. Importantly, the presence of the metastable liquid increases SL formation rates relative to the equivalent one-step pathway, and SL order counterintuitively increases with the rate, revealing a highly desirable and generalizable kinetic strategy to promote and enhance ordered assembly. Copyright © 2024, The Authors. All rights reserved.

关键词： X ray scattering