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An optimized Npro-based method for the expression and purification of intrinsically disordered proteins for an NMR study

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Intrinsically disordered proteins 2015年第1期3卷 e1011004页

作者： Natsuko Goda Naoki Matsuo Takeshi Tenno Sonoko Ishino Yoshizumi Ishino Satoshi Fukuchi Motonori Ota Hidekazu Hiroaki Laboratory of Structural Molecular Pharmacology Graduate School of Pharmaceutical Sciences Nagoya University Furocho Chikusa-ku Nagoya Japan These authors equally contributed to the work. The Structural Biology Research Center and Division of Biological Science Graduate School of Science Furocho Nagoya Japan. Department of Bioscience and Biotechnology Graduate School of Bioresource and Bioenvironmental Sciences and Faculty of Agriculture Kyushu University Fukuoka Japan. Faculty of Engineering Maebashi Institute of Technology Maebashi Japan. Department of Complex Systems Science Graduate School of Information Sciences Nagoya Japan.

Intrinsically disordered proteins (IDPs) are an emerging concept. IDPs have high flexibility in their polypeptide chains, lacking a stable 3-dimensional structure. Because of the difficulty in performing X-ray crystallography for IDPs, nuclear magnetic resonance (NMR) spectroscopy is the first choice for atomic-level investigation of their nature. Given that isotopically labeled IDP samples are necessary for NMR study, a robust and cost-effective protocol for bacterial expression and purification of IDP is also needed. We employed the N (EDDIE)-autoprotease fusion protein system. Although IDPs are believed to be readily degraded by endogenous proteases when expressed in , N-fused IDPs showed excellent resistance to degradation. Seven IDPs of uncharacterized function sampled from the human genome as well as 3 constructs from IDP regions derived from human FancM and Hef were prepared. We improved the protocol of refolding of N (EDDIE) to use dialysis, which is convenient for subsequent purification using reversed-phase (RP) HPLC. The method is robust and widely applicable to any IDP sample, promoting the acquisition of experimental data for IDPs in a high-throughput manner.

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Titelbild: Atomically Precise Nanometer-Sized Pt Catalysts with an Additional Photothermy Functionality (Angew. Chem. 25/2024)

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Angewandte Chemie 2024年第25期136卷

作者： Runguo Wang Dr. Dong Chen Dr. Liang Fang Dr. Wentao Fan Dr. Qing You Guoqing Bian Yue Zhou Dr. Wanmiao Gu Dr. Chengming Wang Dr. Licheng Bai Prof. Dr. Jin Li Prof. Dr. Haiteng Deng Dr. Lingwen Liao Prof. Dr. Jun Yang Prof. Dr. Zhikun Wu Key Laboratory of Materials Physics Anhui Key Laboratory of Nanomaterials and Nanotechnology CAS Center for Excellence in Nanoscience Institute of Solid State Physics HFIPS Chinese Academy of Sciences Hefei 230031 China Key Laboratory of Precision and Intelligent Chemistry University of Science and Technology of China Hefei 230026 P. R. China Institute of Physical Science and Information Technology Anhui University Hefei 230601 P.R. China State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 P. R. China Instruments' Center for Physical Science University of Science and Technology of China Hefei 230026 P. R. China Shenzhen Engineering Center for the Fabrication of Two-Dimensional Atomic Crystals Shenzhen Institutes of Advanced Technology Chinese Academy of Sciences Shenzhen 518055 P. R. China Tsinghua University-Peking University Joint Center for Life Sciences School of Life Sciences Tsinghua University Beijing 100084 P.R.China MOE Key Laboratory of Bioinformatics School of Life Sciences Tsinghua University Beijing 100084 P.R.China

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Atomically Precise Nanometer-Sized Pt Catalysts with an Additional Photothermy Functionality

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Angewandte Chemie 2024年第25期136卷

Atomically precise ~1-nm Pt nanoparticles (nanoclusters, NCs) with ambient stability are important in fundamental research and exhibit diverse practical applications (catalysis, biomedicine, etc.). However, synthesizing such materials is challenging. Herein, by employing the mixture ligand protecting strategy, we successfully synthesized the largest organic-ligand-protected (~1-nm) Pt 23 NCs precisely characterized with mass spectrometry and single-crystal X-ray diffraction analyses. Interestingly, natural population analysis and Bader charge calculation indicate an alternate, varying charge -layer distribution in the sandwich-like Pt 23 NC kernel. Pt 23 NCs can catalyze the oxygen reduction reaction under acidic conditions without requiring calcination and other treatments, and the resulting specific and mass activities without further treatment are sevenfold and eightfold higher than those observed for commercial Pt/C catalysts, respectively. Density functional theory and d -band center calculations interpret the high activity. Furthermore, Pt 23 NCs exhibit a photothermal conversion efficiency of 68.4 % under 532-nm laser irradiation and can be used at least for six cycles, thus demonstrating great potential for practical applications.

关键词： Pt nanocluster atomically precise ambient stability ORR photothermy

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Cover Picture: Atomically Precise Nanometer-Sized Pt Catalysts with an Additional Photothermy Functionality (Angew. Chem. Int. Ed. 25/2024)

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Angewandte Chemie International Edition 2024年第25期63卷

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Publisher's Note: "On Lagrangian single-particle statistics" [Phys. Fluids 24, 055102 (2012)]

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Physics of Fluids 2012年第7期24卷

作者： Falkovich, Gregory Xu, Haitao Pumir, Alain Bodenschatz, Eberhard Biferale, Luca Boffetta, Guido Lanotte, Alessandra S. Toschi, Federico Physics of Complex Systems Weizmann Institute of Science Rehovot 76100 Israel Max Planck Institute for Dynamics and Self-Organization D-37077 Göttingen Germany Laboratoire de Physique Ecole Normale Supérieure de Lyon 46 Université Lyon 1 and CNRS F-69007 Lyon France Institute for Nonlinear Dynamics University of Göttingen D-37077 Göttingen Germany Laboratory of Atomic and Solid State Physics Sibley School of Mechanical and Aerospace Engineering Cornell University Ithaca NY 14853 United States Department of Physics and INFN University of Tor Vergata Via della Ricerca Scientifica 1 I-00133 Roma Italy Department of Physics and INFN University of Torino I-10125 Torino Italy ISAC-CNR Str. Prov. Lecce-Monteroni and INFN Sezione di Lecce I-73100 Lecce Italy Department of Physics Department of Mathematics and Computer Science J.M. Burgerscentrum. Eindhoven University of Technology 5600 MB Eindhoven Netherlands IAC CNR Via dei Taurini 19 I-00185 Roma Italy

This article was originally published online on 14 May 2012 with an incorrectly formatted collaboration and an error in Eq. (9). AIP apologizes for these errors

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Towards provably efficient quantum algorithms for large-scale machine-learning models

arXiv

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arXiv 2023年

作者： Liu, Junyu Liu, Minzhao Liu, Jin-Peng Ye, Ziyu Wang, Yunfei Alexeev, Yuri Eisert, Jens Jiang, Liang Pritzker School of Molecular Engineering The University of Chicago ChicagoIL60637 United States Department of Computer Science The University of Chicago ChicagoIL60637 United States Chicago Quantum Exchange ChicagoIL60637 United States Kadanoff Center for Theoretical Physics The University of Chicago ChicagoIL60637 United States qBraid Co. ChicagoIL60615 United States SeQure ChicagoIL60615 United States Department of Physics The University of Chicago ChicagoIL60637 United States Computational Science Division Argonne National Laboratory LemontIL60439 United States Simons Institute for the Theory of Computing University of California BerkeleyCA94720 United States Department of Mathematics University of California BerkeleyCA94720 United States Center for Theoretical Physics Massachusetts Institute of Technology CambridgeMA02139 United States Martin A. Fisher School of Physics Brandeis University WalthamMA02453 United States Dahlem Center for Complex Quantum Systems Free University Berlin Berlin14195 Germany

Large machine learning models are revolutionary technologies of artificial intelligence whose bottlenecks include huge computational expenses, power, and time used both in the pre-training and fine-tuning process. In this work, we show that fault-tolerant quantum computing could possibly provide provably efficient resolutions for generic (stochastic) gradient descent algorithms, scaling as O(T2 × polylog(n)), where n is the size of the models and T is the number of iterations in the training, as long as the models are both sufficiently dissipative and sparse, with small learning rates. Based on earlier efficient quantum algorithms for dissipative differential equations, we find and prove that similar algorithms work for (stochastic) gradient descent, the primary algorithm for machine learning. In practice, we benchmark instances of large machine learning models from 7 million to 103 million parameters. We find that, in the context of sparse training, a quantum enhancement is possible at the early stage of learning after model pruning, motivating a sparse parameter download and re-upload scheme. Our work shows solidly that faulttolerant quantum algorithms could potentially contribute to most state-of-the-art, large-scale machine-learning problems. Copyright © 2023, The Authors. All rights reserved.

关键词： Differential equations

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Tumor Imaging: Radiopharmaceuticals and Fluorescein Sodium Mediated Triple-Modality Molecular Imaging Allows Precise Image-Guided Tumor Surgery (Adv. Sci. 13/2019)

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Advanced science 2019年第13期6卷 1970081-1970081页

作者： Sheng Zheng Zeyu Zhang Yawei Qu Xiaojun Zhang Hongbo Guo Xiaojing Shi Meishan Cai Caiguang Cao Zhenhua Hu Haifeng Liu Jie Tian Department of Gastroenterology The Third Medical Centre Chinese PLA General Hospital Beijing 100039 China Department of Gastroenterology Anhui No.2 Provincial People's Hospital Hefei 230041 China CAS Key Laboratory of Molecular Imaging Beijing Key Laboratory of Molecular Imaging The State Key Laboratory of Management and Control for Complex Systems Institute of Automation Chinese Academy of Sciences University of Chinese Academy of Sciences Beijing 100190 China School of Life Science and Technology Xidian University Xi'an 710071 China Department of Nuclear Medicine Chinese PLA General Hospital Beijing 100853 China School of Information Sciences and Technology Northwest University Xi'an 710127 China

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Ellipticity control of terahertz high-harmonic generation in a Dirac semimetal

arXiv

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arXiv 2022年

作者： Germanskiy, Semyon Dantas, Renato M.A. Kovalev, Sergey Reinhoffer, Chris Mashkovich, Evgeny A. van Loosdrecht, Paul H.M. Yang, Yunkun Xiu, Faxian Surówka, Piotr Moessner, Roderich Oka, Takashi Wang, Zhe Institute of Physics II University of Cologne Cologne50937 Germany Max Planck Institute for the Physics of Complex Systems Dresden01187 Germany Department of Physics University of Basel Basel4056 Switzerland Institute of Radiation Physics Helmholtz-Zentrum Dresden-Rossendorf Dresden01328 Germany State Key Laboratory of Surface Physics Department of Physics Fudan University Shanghai China Shanghai Qi Zhi Institute No. 701 Yunjin Road Xuhui District Shanghai200232 China Department of Theoretical Physics Wroclaw University of Science and Technology Wroclaw50-370 Poland Institute for Theoretical Physics University of Amsterdam Amsterdam1090 GL Netherlands University of Amsterdam Amsterdam1090 GL Netherlands The Institute for Solid State Physics The University of Tokyo Chiba Kashiwa277-8581 Japan Max Planck Institute for Chemical Physics of Solids Dresden01187 Germany Department of Physics TU Dortmund University Dortmund44227 Germany

We report on terahertz high-harmonic generation in a Dirac semimetal as a function of the driving-pulse ellipticity and on a theoretical study of the field-driven intraband kinetics of massless Dirac fermions. Very efficient control of third-harmonic yield and polarization state is achieved in electron-doped Cd3As2 thin films at room temperature. The observed tunability is understood as resulting from terahertz-field driven intraband kinetics of the Dirac fermions. Our study paves the way for exploiting nonlinear optical properties of Dirac matter for applications in signal processing and optical communications. Copyright © 2022, The Authors. All rights reserved.

关键词： Nonlinear optics

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Magnetic field induced quantum spin liquid in the two coupled trillium lattices of K2Ni2(SO4)3

arXiv

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arXiv 2021年

作者： Dr, Ivica Živković Favre, Virgile Mejia, Catalina Salazar Jeschke, Harald O. Magrez, Arnaud Dabholkar, Bhupen Noculak, Vincent Freitas, Rafael S. Jeong, Minki Hegde, Nagabhushan G. Testa, Luc Babkevich, Peter Su, Yixi Manuel, Pascal Luetkens, Hubertus Baines, Christopher Baker, Peter J. Wosnitza, Jochen Zaharko, Oksana Iqbal, Yasir Reuther, Johannes Rønnow, Henrik M. Laboratory for Quantum Magnetism Institute of Physics École Polytechnique Fédérale de Lausanne LausanneCH-1015 Switzerland Würzburg-Dresden Cluster of Excellence ct.qmat Helmholtz-Zentrum Dresden-Rossendorf Dresden01328 Germany Research Institute for Interdisciplinary Science Okayama University Okayama700-8530 Japan Crystal Growth Facility École Polytechnique Fédérale de Lausanne Lausanne Switzerland group Indian Institute of Technology Madras Chennai600036 India Dahlem Center for Complex Quantum Systems Fachbereich Physik Freie Universität Berlin Berlin14195 Germany Helmholtz-Zentrum für Materialien und Energie Hahn-Meitner-Platz 1 Berlin14109 Germany Instituto de Física Universidade de São Paulo São Paulo05508-090 Brazil School of Physics and Astronomy University of Birmingham Birmingham EdgbastonB15 2TT United Kingdom Forschungszentrum Jülich Lichtenbergstrasse 1 GarchingD-85747 Germany ISIS Pulsed Neutron and Muon Source STFC Rutherford Appleton Laboratory Harwell Science and Innovation Campus Oxfordshire DidcotOX11 0QX United Kingdom Laboratory for Muon Spin Spectroscopy Paul Scherrer Institute VilligenCH-5232 Switzerland Institut für Festkörper- und Materialphysik TU Dresden Dresden01062 Germany Laboratory for Neutron Scattering and Imaging Paul Scherrer Institut VilligenCH-5253 Switzerland

Quantum spin liquids are exotic states of matter which form when strongly frustrated magnetic interactions induce a highly entangled quantum paramagnet far below the energy scale of the magnetic interactions. Three-dimensional cases are especially challenging due to the significant reduction of the influence of quantum fluctuations. Here, we report the magnetic characterization of K2Ni2(SO4)3 forming a three dimensional network of Ni2+ spins. Using density functional theory calculations we show that this network consists of two interconnected spin-1 trillium lattices. In the absence of a magnetic field, magnetization, specific heat, neutron scattering and muon spin relaxation experiments demonstrate a highly correlated and dynamic state, coexisting with a peculiar, very small static component exhibiting a strongly renormalized moment. A magnetic field B & 4 T diminishes the ordered component and drives the system in a pure quantum spin liquid state. This shows that a system of interconnected S = 1 trillium lattices exhibit a significantly elevated level of geometrical frustration. © 2021, CC BY.

关键词： Magnetic fields

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Non-Interacting Ni and Fe Dual-Atom Pair Sites in N-Doped Carbon Catalysts for Efficient Concentrating Solar-Driven Photothermal CO2Reduction

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Angewandte Chemie 2023年第50期135卷

作者： Shengpeng Mo Xinya Zhao Shuangde Li Lili Huang Xin Zhao Quanming Ren Mingyuan Zhang Ruosi Peng Yanan Zhang Xiaobin Zhou Yinming Fan Prof. Qinglin Xie Prof. Yanbing Guo Prof. Daiqi Ye Prof. Yunfa Chen College of Environment Science and Engineering Guilin University of Technology Guilin 541004 P. R. China Key Laboratory of Pesticide & Chemical Biology of Ministry of Education Institute of Environmental and Applied Chemistry College of Chemistry Central China Normal University Wuhan 430079 P. R. China State Key Laboratory of Multi-phase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 P. R. China School of Environment and Energy South China University of Technology Guangzhou 510006 P. R. China College of Geology and Environment Xi'an University of Science and Technology Xi'an 710054 P. R. China School of Environment and Civil Engineering Dongguan University of Technology Dongguan 523808 P. R. China

Solar-to-chemical energy conversion under weak solar irradiation is generally difficult to meet the heat demand of CO 2 reduction. Herein, a new concentrated solar-driven photothermal system coupling a dual-metal single-atom catalyst (DSAC) with adjacent Ni−N 4 and Fe−N 4 pair sites is designed for boosting gas-solid CO 2 reduction with H 2 O under simulated solar irradiation, even under ambient sunlight. As expected, the (Ni, Fe)−N−C DSAC exhibits a superior photothermal catalytic performance for CO 2 reduction to CO (86.16 μmol g −1 h −1 ), CH 4 (135.35 μmol g −1 h −1 ) and CH 3 OH (59.81 μmol g −1 h −1 ), which are equivalent to 1.70-fold, 1.27-fold and 1.23-fold higher than those of the Fe−N−C catalyst, respectively. Based on theoretical simulations, the Fermi level and d-band center of Fe atom is efficiently regulated in non-interacting Ni and Fe dual-atom pair sites with electronic interaction through electron orbital hybridization on (Ni, Fe)−N−C DSAC. Crucially, the distance between adjacent Ni and Fe atoms of the Ni−N−N−Fe configuration means that the additional Ni atom as a new active site contributes to the main *COOH and *HCO 3 dissociation to optimize the corresponding energy barriers in the reaction process, leading to specific dual reaction pathways (COOH and HCO 3 pathways) for solar-driven photothermal CO 2 reduction to initial CO production.

关键词： CO2 Reduction Dual-Single-Atom Catalyst Electronic Interaction Reaction Mechanism Solar

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