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Direct Observation of Mn Distribution/Speciation within and Surrounding a Basidiomycete Fungus in the Production of Mn-Oxides Important in Toxic Element Containment

SSRN

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SSRN 2022年

作者： Takeda, Ayaka Oki, Takumi Yokoo, Hiroki Kawamoto, Keisuke Nakano, Yuriko Ochiai, Asumi Winarni, Ilma Dwi Kitahara, Mitsuki Miyoshi, Kenta Fukuyama, Kenjin Ohara, Yoshiyuki Yamaji, Keiko Ohnuki, Toshihiko Hochella, Michael F. Utsunomiya, Satoshi Department of Chemistry Kyushu University 744 Motooka Nishi-ku Fukuoka819-0395 Japan Ningyo-toge Environmental Engineering Center Japan Atomic Energy Agency 1550 Kamisaibara Tomata-gun Okayama-ken Kagamino-cho708-0601 Japan Graduate School of Life and Environmental Sciences University of Tsukuba 1-1-1 Tennoudai Tsukuba305-8572 Japan Laboratory for Advanced Nuclear Energy Institute of Innovative Research Tokyo Institute of Technology 2-12-1 Ookayama Meguro-ku Tokyo152-8550 Japan Department of Geosciences Virginia Tech BlacksburgVA24061 United States Earth Systems Science Division Energy and Environment Directorate Pacific Northwest National Laboratory RichlandWA99352 United States

Biogenic manganese (Mn) oxides occur ubiquitously in the environment including the uranium (U) mill tailings at the Ningyo-toge U mine in Okayama, Japan, being important in the sequestration of radioactive radium. To understand the nanoscale processes in Mn oxides formation at the U mill tailings site, Mn2+ absorption by a basidiomycete fungus, Coprinopsis urticicola, isolated from Ningyo-toge mine water samples, was investigated in the laboratory under controlled conditions utilizing electron microscopy, synchrotron-based X-ray analysis, and fluorescence microscopy with molecular pH probe. The fungus’ growth was first investigated in an agar-solidified medium supplemented with 1.0 mmol/L of Mn2+, ± Cu2+ (50 – 200 μM), ± Zn2+ (50 – 200 μM), or ± diphenyleneiodonium (DPI) chloride (50 – 100 μM) at 25 ℃. The results revealed that Zn2+ has no significant effects on the Mn oxides formation, whereas Cu2+ and DPI significantly inhibit both fungal growth and Mn oxidation, indicating superoxide-mediated Mn oxidation. Indeed, nitroblue tetrazolium and diaminobenzidine assays on the growing fungus revealed the production of superoxide and peroxide. During the interaction of Mn2+ with the fungus in solution medium at the initial pH of 5.67, a small fraction of Mn2+ infiltrated into the fungal hyphae within 8 h, forming a few tens of nmsized concentrates of soluble Mn2+ in the intracellular pH of ~6.5. After 1 day of incubation, Mn oxides began to precipitate on the hyphae, which were characterized as fibrous nanocrystals with a hexagonal birnessite-structure, these forming spherical aggregates with a diameter of ~1.5 µm. These nanoscale processes associated with the fungal species derived from the Ningyo-toge mine area provide additional insights into the existing mechanisms of Mn oxidation by filamentous fungi at other U mill tailings sites under circumneutral pH conditions. Such processes add to the class of reactions important to the sequestration of toxic elements. © 2022,

关键词： Probes

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Many-core algorithms for high-dimensional gradients on phylogenetic trees

arXiv

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arXiv 2023年

作者： Gangavarapu, Karthik Ji, Xiang Baele, Guy Fourment, Mathieu Lemey, Philippe Matsen, Frederick A. Suchard, Marc A. Department of Biomathematics David Geffen School of Medicine at UCLA University of California Los Angeles United States Department of Mathematics School of Science & Engineering Tulane University New Orleans United States Department of Microbiology Immunology and Transplantation Rega Institute KU Leuven Leuven Belgium Australian Institute for Microbiology and Infection University of Technology Sydney UltimoNSW Australia Public Health Sciences Division Fred Hutchinson Cancer Research Center SeattleWA United States Department of Statistics University of Washington Seattle United States Department of Genome Sciences University of Washington Seattle United States Howard Hughes Medical Institute Fred Hutchinson Cancer Research Center SeattleWA United States Department of Biostatistics Jonathan and Karin Fielding School of Public Health University of California Los Angeles United States Department of Human Genetics David Geffen School of Medicine at UCLA University of California Los Angeles United States Departments of Biostatistics Biomathematics and Human Genetics University of California Los Angeles 695 Charles E. Young Dr. South Los AngelesCA90095-7088 United States

Advancements in high-throughput genomic sequencing are delivering genomic pathogen data at an unprecedented rate, positioning statistical phylogenetics as a critical tool to monitor infectious diseases globally. This rapid growth spurs the need for efficient inference techniques, such as Hamiltonian Monte Carlo (HMC) in a Bayesian framework, to estimate parameters of these phylogenetic models where the dimensions of the parameters increase with the number of sequences N. HMC requires repeated calculation of the gradient of the data log-likelihood with respect to (wrt) all branch-length-specific (BLS) parameters that traditionally takes O(N2) operations using the standard pruning algorithm. A recent study proposes an approach to calculate this gradient in O(N), enabling researchers to take advantage of gradient-based samplers such as HMC. The CPU implementation of this approach makes the calculation of the gradient computationally tractable for nucleotide-based models but falls short in performance for larger state-space size models, such as Markov-modulated and codon models. Here, we describe novel massively parallel algorithms to calculate the gradient of the log-likelihood wrt all BLS parameters that take advantage of graphics processing units (GPUs) and result in many fold higher speedups over previous CPU implementations. We benchmark these GPU algorithms on three computing systems using three evolutionary inference examples exploring complete genomes from 997 dengue viruses, 62 carnivore mitochondria and 49 yeasts, and observe a greater than 128-fold speedup over the CPU implementation for codon-based models and greater than 8-fold speedup for nucleotide-based models. As a practical demonstration, we also estimate the timing of the first introduction of West Nile virus into the continental Unites States under a codon model with a relaxed molecular clock from 104 full viral genomes, an inference task previously intractable. We provide an implementation of our GP

关键词： Phylogenetic

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Publisher Correction: Unconventional excitonic states with phonon sidebands in layered silicon diphosphide

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Nature materials 2022年第10期21卷 1212页

作者： Ling Zhou Junwei Huang Lukas Windgaetter Chin Shen Ong Xiaoxu Zhao Caorong Zhang Ming Tang Zeya Li Caiyu Qiu Simone Latini Yangfan Lu Di Wu Huiyang Gou Andrew T S Wee Hideo Hosono Steven G Louie Peizhe Tang Angel Rubio Hongtao Yuan National Laboratory of Solid State Microstructures Jiangsu Key Laboratory of Artificial Functional Materials College of Engineering and Applied Sciences and Collaborative Innovation Center of Advanced Microstructures Nanjing University Nanjing China. Max Planck Institute for the Structure and Dynamics of Matter Center for Free Electron Laser Science Hamburg Germany. Department of Physics University of California Berkeley CA USA. Materials Sciences Division Lawrence Berkeley National Laboratory Berkeley CA USA. School of Materials Science and Engineering Peking University Beijing China. Materials Research Center for Element Strategy Tokyo Institute of Technology Yokohama Japan. College of Materials Science and Engineering National Engineering Research Center for Magnesium Alloys Chongqing University Chongqing China. Center for High Pressure Science and Technology Advanced Research Beijing China. Department of Physics National University of Singapore Singapore Singapore. Max Planck Institute for the Structure and Dynamics of Matter Center for Free Electron Laser Science Hamburg Germany. peizhet@***. School of Materials Science and Engineering Beihang University Beijing China. peizhet@***. Max Planck Institute for the Structure and Dynamics of Matter Center for Free Electron Laser Science Hamburg Germany. angel.rubio@mpsd.mpg.de. Center for Computational Quantum Physics Simons Foundation Flatiron Institute New York NY USA. angel.rubio@mpsd.mpg.de. National Laboratory of Solid State Microstructures Jiangsu Key Laboratory of Artificial Functional Materials College of Engineering and Applied Sciences and Collaborative Innovation Center of Advanced Microstructures Nanjing University Nanjing China. htyuan@***.

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Cocreating the Visualization of Digital Mobility Outcomes: Delphi-Type Process With Patients

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JMIR Formative research 2025年 9卷 e68782页

作者： Lumsdon, Jack Wilson, Cameron Alcock, Lisa Becker, Clemens Benvenuti, Francesco Bonci, Tecla van den Brande, Koen Brittain, Gavin Brown, Philip Buckley, Ellen Caruso, Marco Caulfield, Brian Cereatti, Andrea Delgado-Ortiz, Laura Del Din, Silvia Evers, Jordi Garcia-Aymerich, Judith Gaßner, Heiko Gur Arieh, Tova Hansen, Clint Hausdorff, Jeffrey M. Hiden, Hugo Hume, Emily Kirk, Cameron Maetzler, Walter Megaritis, Dimitrios Rochester, Lynn Scott, Kirsty Sharrack, Basil Sutton, Norman Vereijken, Beatrix Vogiatzis, Ioannis Yarnall, Alison Keogh, Alison Cantu, Alma Population Health Sciences Institute Faculty of Medical Sciences Newcastle University Newcastle Upon Tyne United Kingdom School of Clinical Medicine Department of Public Health and Primary Care University of Cambridge Cambridge United Kingdom Translational and Clinical Research Institute Faculty of Medical Sciences Newcastle University Newcastle Upon Tyne United Kingdom NIHR Newcastle Biomedical Research Centre Newcastle University The Newcastle Upon Tyne Hospitals NHS Foundation Trust Newcastle upon Tyne United Kingdom Robert Bosch Society for Medical Research Stuttgart Germany Digital Geriatrics Unit Medical Centre University of Heidelberg Heidelberg Germany Mobilise-D Patient and Public Advisory Group Newcastle Upon Tyne United Kingdom School of Mechanical Aerospace and Civil Engineering University of Sheffield Sheffield United Kingdom Insigneo Institute for Silico Medicine University of Sheffield Sheffield United Kingdom Department of Neuroscience Sheffield NIHR Translational Neuroscience BRC Sheffield Teaching Hospitals NHS Foundation Trust Sheffield United Kingdom Sheffield Institute for Translational Neuroscience University of Sheffield Sheffield United Kingdom The Newcastle Upon Tyne Hospitals NHS Foundation Trust Newcastle Upon Tyne United Kingdom Division of Clinical Medicine University of Sheffield Sheffield United Kingdom Department of Electronics and Telecommunications Politecnico di Torino Turin Italy Insights Centre Data Analytics University College Dublin Dublin Ireland School of Public Health Physiotherapy and Sports Science University of College Dublin Dublin Ireland Barcelona Institute for Global Health Barcelona Spain Department of Medicine and Life Sciences Pompeu Fabra University Barcelona Spain Center for Biomedical Research Madrid Spain McRoberts BV The Hague Netherlands Department of Molecular Neurology University Hospital Erlangen Erlangen Germany Fraunhofer Institute for Integrated Circuits IIS Erlangen Germany Departmen

Background: Recent technological advances in wearable devices offer new potential for measuring mobility in real-world contexts. Mobilise-D has validated digital mobility outcomes to provide novel outcomes and end points in clinical research of 4 different long-term health conditions (Parkinson disease, multiple sclerosis, chronic obstructive pulmonary disease, and proximal femoral fracture). These outcomes also provide unique information that is important to patients;however, there is limited literature that explores the optimal methods to achieve this, such as the best way to visualize patients’ data. Objective: This study aimed to identify meaningful outcomes for each condition and how to best visualize them from the perspective of end users. Methods: Using a Delphi-type protocol with patients as subject matter experts, we gathered iterative feedback on the cocreation of visualizations through 3 rounds of questionnaires. An open-ended questionnaire was used in round 1 to understand what aspects of mobility were most influenced by their health condition. These responses were mapped onto relevant digital mobility outcomes and walking experiences and then prioritized for visualization. Using patient responses, we worked alongside researchers, clinicians, and a patient advisory group to develop visualizations that depicted a week of mobility data. During rounds 2 and 3, participants rated usefulness and ease of understanding on a 5-point Likert scale and provided unstructured feedback in comment boxes for each visualization. Visualizations were refined using the feedback from round 2 before receiving further feedback in round 3. Results: Participation varied across rounds 1 to 3 (n=48, n=79, and n=78, respectively). Round 1 identified important outcomes and contexts for each health condition, such as walking speed and stride length for people with Parkinson disease or multiple sclerosis and number of steps for people with chronic obstructive pulmonary disease or prox

关键词： cocreation data visualization digital mobility outcomes mobility wearable devices

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Dimensional control of octahedral tilt in SrRuO3 via infinite-layered oxides

arXiv

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arXiv 2021年

作者： Lin, Shan Zhang, Qinghua Sang, Xiahan Zhao, Jiali Cheng, Sheng Huon, Amanda Jin, Qiao Chen, Shuang Chen, Shengru Guo, Haizhong He, Meng Ge, Chen Wang, Can Wang, Jia-Ou Fitzsimmons, Michael R. Gu, Lin Zhu, Tao Jin, Kui-Juan Guo, Er-Jia Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing100190 China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing100049 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Nanostructure Research Center Wuhan University of Technology 122 Luoshi Rd. Wuhan430070 China Institute of High Energy Physics Chinese Academy of Sciences Beijing100049 China Spallation Neutron Source Science Center Dongguan523803 China School of Physical Sciences University of Chinese Academy of Sciences Beijing100190 China Neutron Scattering Division Oak Ridge National Laboratory Oak RidgeTN37831 United States School of Physical Engineering Zhengzhou University Zhengzhou450001 China Songshan Lake Materials Laboratory DongguanGuangdong523808 China

Manipulation of octahedral distortion at atomic length scale is an effective means to tune the physical ground states of functional oxides. Previous work demonstrates that epitaxial strain and film thickness are variable parameters to modify the octahedral rotation and tilt. However, selective control of bonding geometry by structural propagation from adjacent layers is rarely studied. Here we propose a new route to tune the ferromagnetic response in SrRuO3 (SRO) ultrathin layers by oxygen coordination of adjacent SrCuO2 (SCO) layers. The infinite-layered CuO2 in SCO exhibits a structural transformation from "planar-type" to "chain-type" as reducing film thickness. These two orientations dramatically modify the polyhedral connectivity at the interface, thus altering the octahedral distortion of SRO. The local structural variation changes the spin state of Ru and hybridization strength between Ru 4d and O 2p orbitals, leading to a significant change in the magnetoresistance and anomalous Hall resistivity of SRO layers. These findings could launch further investigations into adaptive control of magnetoelectric properties in quantum oxide heterostructures using oxygen coordination. © 2021, CC BY.

关键词： Ruthenium compounds

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What-if Scenario Analysis for IT Services in Hybrid Cloud Environments with BDMaaS+

What-if Scenario Analysis for IT Services in Hybrid Cloud En...

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IFIP/IEEE International Symposium on Integrated Network Management

作者： Walter Cerroni Luca Foschini Genady Ya. Grabarnik Larisa Shwartz Mauro Tortonesi Department of Electrical University of Bologna Bologna Italy Department of Computer Science and Engineering University of Bologna Bologna Italy Department of Mathematics and Computer Science St. John’s University Queens NY USA Operational Innovation IBM TJ Watson Research Center NY USA Department of Mathematics and Computer Science University of Ferrara Ferrara Italy

ISBN: (纸本)9781728106182;9783903176157

The high sophistication of IT services, more and more often operated over distributed hybrid Cloud environments, makes it extremely difficult to evaluate the impact of changes at the business level over service architecture before deploying them. The performance assessment of possible alternative deployments calls for decision support tools to enable what-if scenario analysis, which requires also to adopt realistic Cloud network models, currently not available. To fill that gap, this paper illustrates the potential of our Business-Driven Management as a Service Plus (BDMaaS+) support that eases management operations in the above context, and presents a thorough experimental evaluation of our solution. Collected results demonstrate how a service provider can leverage BDMaaS+ to explore the potential of high-level business Service Level Agreement (SLA) changes and data center additions to optimize the performance of an enterprise class IT service deployed, in a realistic hybrid Cloud environment, before (re-)enacting them.

关键词： Cloud computing Data centers Business computer architecture Software Tools Optimization

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Correction to: A digital rights management system based on a scalable blockchain

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Peer-to-Peer Networking and Applications 2021年第4期14卷 1869-1869页

作者： Garba, Abba Dwivedi, Ashutosh Dhar Kamal, Mohsin Srivastava, Gautam Tariq, Muhammad Hasan, M. Anwar Chen, Zhong Key Laboratory of High Confidence Software Technologies Peking University MoE Beijing China Department of Computer Science and Technology EECS Peking University Beijing China Department of Applied Mathematics and Computer Science Technical University of Denmark Lyngby Denmark Department of Electrical Engineering National University of Computer and Emerging Sciences Peshawar Pakistan Department of Mathematics and Computer Science Brandon University Brandon Canada Research Center for Interneural Computing China Medical University Taichung Republic of China Princeton University Princeton USA Department of Electrical and Computer Engineering University of Waterloo Waterloo Canada

A Correction to this paper has been published: https://***/10.1007/s12083-021-01098-2

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Searching for gravitational wave optical counterparts with the Zwicky Transient Facility: summary of O4a

arXiv

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arXiv 2024年

作者： Ahumada, Tomás Anand, Shreya Coughlin, Michael W. Gupta, Vaidehi Kasliwal, Mansi M. Karambelkar, Viraj R. Stein, Robert D. Waratkar, Gaurav Swain, Vishwajeet Jegou du Laz, Theophile Anumarlapudi, Akash Andreoni, Igor Bulla, Mattia Srinivasaragavan, Gokul P. Toivonen, Andrew Wold, Avery Bellm, Eric C. Cenko, S. Bradley Kaplan, David L. Sollerman, Jesper Bhalerao, Varun Perley, Daniel Salgundi, Anirudh Suresh, Aswin Hinds, K.-Ryan Reusch, Simeon Necker, Jannis Cook, David O. Pletskova, Natalya Singer, Leo P. Banerjee, Smaranika Barna, Tyler Copperwheat, Christopher M. Healy, Brian Kiendrebeogo, R. Weizmann Kumar, Harsh Kumar, Ravi Pezzella, Marianna Sagués-Carracedo, Ana Sravan, Niharika Bloom, Joshua S. Chen, Tracy X. Graham, Matthew Helou, George Laher, Russ R. Mahabal, Ashish A. Purdum, Josiah Anupama, G.C. Barway, Sudhanshu Basu, Judhajeet Raman, Dhananjay Roychowdhury, Tamojeet Division of Physics Mathematics and Astronomy California Institute of Technology PasadenaCA91125 United States School of Physics and Astronomy University of Minnesota MinneapolisMN55455 United States Department of Physics Indian Institute of Technology West Bengal Kharagpur721302 India Department of Physics Indian Institute of Technology Bombay Powai 400 076 India Department of Physics University of Wisconsin-Milwaukee P.O. Box 413 MilwaukeeWI53201 United States Joint Space-Science Institute University of Maryland College ParkMD20742 United States Department of Astronomy University of Maryland College ParkMD20742 United States Astrophysics Science Division NASA Goddard Space Flight Center MC 661 GreenbeltMD20771 United States Department of Physics and Earth Science University of Ferrara via Saragat 1 FerraraI-44122 Italy INFN Sezione di Ferrara via Saragat 1 FerraraI-44122 Italy INAF Osservatorio Astronomico d’Abruzzo via Mentore Maggini snc Teramo64100 Italy IPAC California Institute of Technology 1200 E. California Blvd PasadenaCA91125 United States DIRAC Institute Department of Astronomy University of Washington 3910 15th Avenue NE SeattleWA98195 United States The Oskar Klein Centre Department of Astronomy Albanova Stockholm University StockholmSE-106 91 Sweden Astrophysics Research Institute Liverpool John Moores University IC2 Liverpool Science Park 146 Brownlow Hill LiverpoolL3 5RF United Kingdom Deutsches Elektronen-Synchrotron DESY Platanenallee 6 Zeuthen15738 Germany Department of Physics Drexel University PhiladelphiaPA19104 United States Astrophysics Research Institute IC2 Liverpool Science Park 146 Brownlow Hill LiverpoolL3 5RF United Kingdom Laboratoire de Physique et de Chimie de l’Environnement Université Joseph KI-ZERBO Ouagadougou Burkina Faso Artemis Observatoire de la Côte d’Azur Université Côte d’Azur Boulevard de l’Observatoire NiceF-06304 France Department of Physics Indian Institute o

During the first half of the fourth observing run (O4a) of the International Gravitational Wave Network (IGWN), the Zwicky Transient Facility (ZTF) conducted a systematic search for kilonova (KN) counterparts to binary neutron star (BNS) and neutron star–black hole (NSBH) merger candidates. Here, we present a comprehensive study of the five high-significance (False Alarm Rate less than 1 per year) BNS and NSBH candidates in O4a. Our follow-up campaigns relied on both target-of-opportunity observations (ToO) and re-weighting of the nominal survey schedule to maximize coverage. We describe the toolkit we have been developing, Fritz, an instance of SkyPortal, instrumental in coordinating and managing our telescope scheduling, candidate vetting, and follow-up observations through a user-friendly interface. ZTF covered a total of 2841 deg2 within the skymaps of the high-significance GW events, reaching a median depth of g ≈ 20.2 mag. We circulated 15 candidates, but found no viable KN counterpart to any of the GW events. Based on the ZTF non-detections of the high-significance events in O4a, we used a Bayesian approach, nimbus, to quantify the posterior probability of KN model parameters that are consistent with our non-detections. Our analysis favors KNe with initial absolute magnitude fainter than -16 mag. The joint posterior probability of a GW170817-like KN associated with all our O4a follow-ups was 64%. Additionally, we use a survey simulation software, simsurvey, to determine that our combined filtered efficiency to detect a GW170817-like KN is 36%, when considering the 5 confirmed astrophysical events in O3 (1 BNS and 4 NSBH events), along with our O4a follow-ups. Following Kasliwal et al. (2020), we derived joint constraints on the underlying KN luminosity function based on our O3 and O4a follow-ups, determining that no more than 76% of KNe fading at 1 mag day-1 can peak at a magnitude brighter than -17.5 mag. Copyright © 2024, The Authors. All rights reserved.

关键词： Gravity waves

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Ultrahigh-pressure form of SiO2 glass with dense pyrite-type crystalline homology

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Physical Review B 2019年第4期99卷 045153-045153页

作者： M. Murakami S. Kohara N. Kitamura J. Akola H. Inoue A. Hirata Y. Hiraoka Y. Onodera I. Obayashi J. Kalikka N. Hirao T. Musso A. S. Foster Y. Idemoto O. Sakata Y. Ohishi Department of Earth Sciences ETH Zürich Zürich 8092 Switzerland Department of Earth and Planetary Materials Science Tohoku University Sendai 980-8578 Japan Research Center for Advanced Measurement and Characterization National Institute for Materials Science (NIMS) Hyogo 679-5148 Japan Center for Materials research by Information Integration (CMI2) Research and Services Division of Materials Data and Integrated System (MaDIS) NIMS Ibaraki 305-0047 Japan Research and Utilization Division Japan Synchrotron Radiation Research Institute Hyogo 679-5198 Japan School of Materials Science Japan Advanced Institute of Science and Technology Ishikawa 923-1211 Japan PRESTO Japan Science and Technology Agency Tokyo 102-0076 Japan Department of Pure and Applied Chemistry Faculty of Science and Technology Tokyo University of Science Chiba 278-8510 Japan Department of Physics Tampere University of Technology FI-33101 Tampere Finland Department of Physics Norwegian University of Science and Technology NO-7481 Trondheim Norway Institute of Industrial Science The University of Tokyo Tokyo 153-8505 Japan Graduate School of Fundamental Science and Engineering Waseda University Tokyo 169-8555 Japan Kagami Memorial Research Institute for Materials Science and Technology Waseda University Tokyo 169-0051 Japan Mathematics for Advanced Materials-OIL AIST Sendai 980-8577 Japan WPI Advanced Institute for Materials Research Tohoku University Sendai 980-8577 Japan Kyoto University Institute for Advanced Study Kyoto University Kyoto 606-8501 Japan Center for Advanced Intelligence Project RIKEN Tokyo 103-0027 Japan Institute for Integrated Radiation and Nuclear Science Kyoto University Osaka 590-0494 Japan Department of Applied Physics Aalto University FI-00076 Aalto Finland Division of Electrical Engineering and Computer Science Graduate School of Natural Science and Technology Kanazawa University Kanazawa 920-1192 Japan

High-pressure synthesis of denser glass has been a longstanding interest in condensed-matter physics and materials science because of its potentially broad industrial application. Nevertheless, understanding its nature under extreme pressures has yet to be clarified due to experimental and theoretical challenges. Here we reveal the formation of OSi4 tetraclusters associated with that of SiO7 polyhedra in SiO2 glass under ultrahigh pressures to 200 gigapascal confirmed both experimentally and theoretically. Persistent homology analyses with molecular dynamics simulations found increased packing fraction of atoms whose topological diagram at ultrahigh pressures is similar to a pyrite-type crystalline phase, although the formation of tetraclusters is prohibited in the crystalline phase. This critical difference would be caused by the potential structural tolerance in the glass for distortion of oxygen clusters. Furthermore, an expanded electronic band gap demonstrates that chemical bonds survive at ultrahigh pressure. This opens up the synthesis of topologically disordered dense oxide glasses.

关键词： Chemical bonding Density of states Electronic structure Phase transitions Pressure effects Specific phase transitions Structural properties Topological phase transition Topological phases of matter Density functional theory Molecular dynamics Wannier function methods X-ray diffraction X-ray powder diffraction

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The forefront of chemical engineering research

Nature Chemical Engineering

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Nature Chemical engineering 2024年第1期1卷 18-27页

作者： Laura Torrente-Murciano Jennifer B. Dunn Panagiotis D. Christofides Jay D. Keasling Sharon C. Glotzer Sang Yup Lee Kevin M. Van Geem Jean Tom Gaohong He Department of Chemical Engineering and Biotechnology University of Cambridge Cambridge UK Chemical and Biological Engineering Center for Engineering Sustainability and Resilience Northwestern University Evanston IL USA Department of Chemical and Biomolecular Engineering University of California Los Angeles Los Angeles CA USA Department of Chemical & Biomolecular Engineering University of California Berkeley Berkeley CA USA Department of Bioengineering University of California Berkeley Berkeley CA USA California Institute of Quantitative Biosciences (QB3) University of California Berkeley Berkeley CA USA Division of Biological Systems and Engineering Lawrence Berkeley National Laboratory Berkeley CA USA Joint BioEnergy Institute Emeryville CA USA Center for Biosustainability Danish Technical University Lyngby Denmark Center for Synthetic Biochemistry Shenzhen Institutes for Advanced Technologies Shenzhen China Department of Chemical Engineering University of Michigan Ann Arbor MI USA Metabolic and Biomolecular Engineering National Research Laboratory Systems Metabolic Engineering and Systems Healthcare Cross-Generation Collaborative Laboratory Department of Chemical and Biomolecular Engineering (BK21 four) BioProcess Engineering Research Center Korea Advanced Institute of Science and Technology (KAIST) Daejeon Republic of Korea Laboratory for Chemical Technology Department of Materials Textiles and Chemical Engineering Faculty of Engineering and Architecture Ghent University Ghent Belgium Chemical Process Development Global Product Development and Supply Bristol Myers Squibb New Brunswick NJ USA State Key Laboratory of Fine Chemicals R&D Center of Membrane Science and Technology School of Chemical Engineering Panjin Institute of Industrial Technology Liaoning Key Laboratory of Chemical Additive Synthesis and Separation Dalian University of Technology Dalian Liaoning China

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