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Transforming Red Phosphorus Photocatalysis: Dual Roles of Pre-Anchored Ru Single Atoms in Defect and Interface engineering

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Angewandte Chemie 2024年第45期136卷

作者： Junwei Bian Wei Zhang Prof. Yun Hau Ng Prof. Zhuofeng Hu Prof. Zhen Wei Yuxi Liu Prof. Jiguang Deng Prof. Hongxing Dai Prof. Lin Jing Beijing Key Laboratory for Green Catalysis and Separation College of Materials Science and Engineering Beijing University of Technology Beijing 100124 China School of Energy and Environment City University of Hong Kong Tat Chee Avenue Kowloon 999077 Hong Kong S.A.R. China Chemical Engineering Program Physical Science and Engineering Division King Abdullah University of Science and Technology Thuwal 23955-6900 Kingdom of Saudi Arabia School of Environmental Science and Engineering Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology Sun Yat-sen University Guangzhou 510275 China

Crystalline red phosphorus (CRP), known for its promising photocatalytic properties, faces challenges in photocatalytic hydrogen evolution (PHE) due to undesired inherent charge deep trapping and recombination effects induced by defects. This study overcomes these limitations through an innovative strategy in integrating ruthenium single atoms (Ru 1 ) within CRP to simultaneously repair the intrinsic undesired vacancy defects and serve as the uniformly distributed anchoring sites for a controllable growth into ruthenium nanoparticles (Ru NP ). Hence, a highly functionalized CRP with Ru 1 and Ru NP (Ru 1-NP /CRP) with concerted effects in regulating electronic structures and promoting interfacial charge transfer has been achieved. Advanced characterizations unveil the pioneering dual role of pre-anchored Ru 1 (analogous to the “Tai Chi” principle) in transforming CRP photocatalysis. The regulations of vacancy defects on the surface of CRP minimize the detrimental deep charge trapping, resulting in the prolonged lifetime of active charges. With the well-distributed in situ growth of Ru NP on Ru 1 sites, the constructed robust “bridge” that connects CRP and Ru NP facilitates constructive interfacial charge transfer. Ultimately, the synergistic effect induced by the pre-anchored Ru 1 endows Ru 1-NP /CRP with an exceptional PHE rate of 3175 μmol h −1 g −1 , positioning it as one of the most efficient elemental-based photocatalysts available. This breakthrough underscores the crucial role of pre-anchoring metal single atoms at defect sites of catalysts in enhancing sustainable hydrogen production.

关键词： photocatalytic hydrogen evolution red phosphorus ruthenium single atom defect engineering interface engineering

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Defective corticomuscular connectivity during walking in patients with Parkinson's disease (vol 124, pg 1399, 2020)

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JOURNAL OF NEUROPHYSIOLOGY 2020年第6期124卷 2076-2076页

作者： Yokoyama, H. Yoshida, T. Zabjek, K. Chen, R. Masani, K. Rehabilitation Engineering Laboratory Toronto Rehabilitation Institute University Health Network Toronto Ontario Canada Department of Electrical and Electronic Engineering Tokyo University of Agriculture and Technology Tokyo Japan Applied Rehabilitation Technology Lab (ART-Lab) University Medical Center Göttingen Göttingen Germany Department of Physical Therapy University of Toronto Toronto Ontario Canada Division of Neurology Department of Medicine University of Toronto Toronto Ontario Canada Krembil Research Institute University Health Network Toronto Ontario Canada Edmond J. Safra Program in Parkinson’s Disease University Health Network Toronto Ontario Canada Rehabilitation Engineering Laboratory Toronto Rehabilitation Institute University Health Network Toronto Ontario Canada Institute of Biomaterials and Biomedical Engineering University of Toronto Toronto Ontario Canada

Gait disturbances are common in individuals with Parkinson’s disease (PD). Although the basic patterns of walking are thought to be controlled by the brainstem and spinal networks, recent studies have found significant corticomuscular coherence in healthy individuals during walking. However, it still remains unknown how PD affects the cortical control of muscles during walking. As PD typically develops in older adults, it is important to investigate the effects of both aging and PD when examining disorders in patients with PD. Here, we assessed the effects of PD and aging on corticomuscular communication during walking by investigating corticomuscular coherence. We recorded electroencephalographic and electromyographic signals in 10 individuals with PD, 9 healthy older individuals, and 15 healthy young individuals. We assessed the corticomuscular coherence between the motor cortex and two lower leg muscles, tibialis anterior (TA) and medial gastrocnemius, during walking. Older and young groups showed sharp peaks in muscle activation patterns at specific gait phases, whereas the PD group showed prolonged patterns. Smaller corticomuscular coherence was found in the PD group compared with the healthy older group in the α band (8−12 Hz) for both muscles, and in the β band (16−32 Hz) for TA. Older and young groups did not differ in the magnitude of corticomuscular coherence. Our results indicated that PD decreased the corticomuscular coherence during walking, whereas it was not affected by aging. This lower corticomuscular coherence in PD may indicate lower-than-normal corticomuscular communication, although direct or indirect communication is unknown, and may cause impaired muscle control during *** & NOTEWORTHY Mechanisms behind how Parkinson’s disease (PD) affects cortical control of muscles during walking remain unclear. As PD typically develops in the elderly, investigation of aging effects is important to examine deficits regarding PD. Here, we demonstrated

关键词： aging electromyography motor cortex Parkinson’s disease walking

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AI-driven 3D Spatial Transcriptomics

arXiv

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arXiv 2025年

作者： Almagro-Pérez, Cristina Song, Andrew H. Weishaupt, Luca Kim, Ahrong Jaume, Guillaume Williamson, Drew F.K. Hemker, Konstantin Lu, Ming Y. Singh, Kritika Chen, Bowen Le, Long Phi Baras, Alexander S. Jiang, Sizun Bashashati, Ali Liu, Jonathan T.C. Mahmood, Faisal Department of Pathology Mass General Brigham Harvard Medical School BostonMA United States Cancer Program Broad Institute of Harvard and MIT CambridgeMA United States Data Science Program Dana-Farber Cancer Institute BostonMA United States Harvard-MIT Division of Health Sciences and Technology Massachusetts Institute of Technology CambridgeMA United States Department of Pathology Pusan National University Busan Korea Republic of Department of Pathology and Laboratory Medicine Emory University School of Medicine AtlantaGA United States Department of Computer Science & Technology University of Cambridge Cambridge United Kingdom Department of Electrical Engineering and Computer Science Massachusetts Institute of Technology CambridgeMA United States Rutgers Robert Wood Johnson Medical School New BrunswickNJ United States Department of Pathology Johns Hopkins Hospital BaltimoreMD United States Department of Biomedical Engineering Johns Hopkins Hospital BaltimoreMD United States Broad Institute of Harvard and MIT CambridgeMA United States Center for Virology and Vaccine Research Beth Israel Deaconess Medical Center Harvard Medical School BostonMA United States Department of Pathology Dana Farber Cancer Institute BostonMA United States Department of Pathology and Laboratory Medicine University of British Columbia VancouverBC Canada School of Biomedical Engineering University of British Columbia VancouverBC Canada Department of Mechanical Engineering Bioengineering Laboratory Medicine & Pathology University of Washington SeattleWA United States Harvard Data Science Initiative Harvard University CambridgeMA United States

A comprehensive three-dimensional (3D) map of tissue architecture and gene expression is crucial for illuminating the complexity and heterogeneity of tissues across diverse biomedical applications1. However, most spatial transcriptomics (ST) approaches remain limited to two-dimensional (2D) sections of tissue2–4. Although current 3D ST methods hold promise, they typically require extensive tissue sectioning, are complex, are not compatible with non-destructive 3D tissue imaging technologies, and often lack scalability5–8. Here, we present VOlumetrically Resolved Transcriptomics EXpression (VORTEX), an AI framework that leverages 3D tissue morphology and minimal 2D ST to predict volumetric 3D ST. By pretraining on diverse 3D morphology–transcriptomic pairs from heterogeneous tissue samples and then fine-tuning on minimal 2D ST data from a specific volume of interest, VORTEX learns both generic tissue-related and sample-specific morphological correlates of gene expression. This approach enables dense, high-throughput, and fast 3D ST, scaling seamlessly to large tissue volumes far beyond the reach of existing 3D ST techniques. By offering a cost-effective and minimally destructive route to obtaining volumetric molecular insights, we anticipate that VORTEX will accelerate biomarker discovery and our understanding of morphomolecular associations and cell states in complex tissues. Interactive 3D ST volumes can be viewed at https://***/. © 2025, CC BY-NC-ND.

关键词： Vortex flow

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EXPPO: EXecution Performance Profiling and Optimization for CPS Co-simulation-as-a-Service

EXPPO: EXecution Performance Profiling and Optimization for ...

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International Symposium on Object-Oriented Real-Time Distributed Computing

作者： Yogesh D. Barve Himanshu Neema Zhuangwei Kang Hongyang Sun Aniruddha Gokhale Thomas Roth Department of Electrical Engineering and Computer Science Vanderbilt University Nashville TN USA Smart Grid and Cyber-Physical Systems Program Office Engineering Laboratory National Institute of Standards and Technology Gaithersburg MD USA

ISBN: (数字)9781728169583

ISBN: (纸本)9781728169590

A co-simulation may comprise several heterogeneous federates with diverse spatial and temporal execution characteristics. In an iterative time-stepped simulation, a federation exhibits the Bulk Synchronous Parallel (BSP) computation paradigm in which all federates perform local operations and synchronize with their peers before proceeding to the next round of computation. In this context, the lowest performing (i.e., slowest) federate dictates the progression of the federation logical time. One challenge in co-simulation is performance profiling for individual federates and entire federations. The computational resource assignment to the federates can have a large impact on federation performance. Furthermore, a federation may comprise federates located on different physical machines as is the case for cloud and edge computing environments. As such, distributed profiling and resource assignment to the federation is a major challenge for operationalizing the co-simulation execution at scale. This paper presents the Execution Performance Profiling and Optimization (EXPPO) methodology, which addresses these challenges by using execution performance profiling at each simulation execution step and for every federate in a federation. EXPPO uses profiling to learn performance models for each federate, and uses these models in its federation resource recommendation tool to solve an optimization problem that improves the execution performance of the co-simulation. Using an experimental testbed, the efficacy of EXPPO is validated to show the benefits of performance profiling and resource assignment in improving the execution runtimes of co-simulations while also minimizing the execution cost.

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High-temperature mid-IR absorption and reaction kinetics of 2-methyl-1,3-dioxolane: An experimental and theoretical study

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Journal of Photochemistry and Photobiology 2023年 13卷

作者： Adil, Mohammad Giri, Binod Raj Mai, Tam V.-T. Szőri, Milán Huynh, Lam K. Farooq, Aamir Mechanical Engineering Program Physical Science and Engineering Division King Abdullah University of Science and Technology (KAUST) Thuwal 23955-6900 Saudi Arabia KAUST Clean Combustion Research Center King Abdullah University of Science and Technology Saudi Arabia Molecular Science and Nano-Materials Lab Institute for Computational Science and Technology SBI Building Quang Trung Software City Tan Chanh Hiep Ward District 12 Ho Chi Minh Viet Nam University of Science Vietnam National University – HCMC 227 Nguyen Van Cu Ward 4 District 5 Ho Chi Minh Viet Nam Vietnam National University – HCMC Quarter 6 Linh Trung Ward Thu Duc Ho Chi Minh Viet Nam Institute of Chemistry University of Miskolc Egyetemváros A/2 Miskolc H-3515 Hungary School of Chemical and Environmental Engineering International University Quarter 6 Linh Trung Ward Thu Duc City Ho Chi Minh City Viet Nam

This work reports the mid-IR spectroscopy and reaction kinetics of 2-methyl-1,3-dioxolane (2M13DO). We carried out spectroscopic measurements to deduce temperature-dependent absorption cross-sections of 2M13DO over a broad wavelength range of 8.4–10.5 μm (950–1190 cm⁻¹). For these measurements, we employed a rapidly tuning MIRcat-QT™ laser that can be operated either at a fixed wavelength or scanned mode over wide wavelength regions. By operating the laser at a fixed wavelength, we monitored the decay of 2M13DO behind reflected shock waves over T₅ = 1050–1400 K and P₅ = 0.7 and 2.6 bar. Our measured concentration time-histories of 2M13DO allowed us to directly extract the overall rate coefficients for the unimolecular decomposition of 2M13DO using the first-order rate law. We did not observe any pressure dependence in the measured rate coefficients, indicating that the reaction is close to the high-pressure limit. By employing the W1U composite method, we explored the important pyrolysis reaction pathways of 2M13DO in the reactive potential energy surface. Three important reaction channels, namely, 2M13DO → CH₂[dbnd]CHOCH₂CH₂OH (IM1), 2M13DO → 2CH₃CHO (P3), 2M13DO → CH₃ + 1,3-dioxolan-2-yl (P4) were identified. Below 700 K, IM1 forming channel is dominant, whereas CH₃CHO formation is dominant under our experimental conditions. Above 1500 K, the radical forming channel (CH₃+P4) takes over other channels. At higher temperatures, the contribution of the radical forming channel continually increases, accounting for ∼ 99% at 2000 K. We used the stochastic RRKM-ME model to predict the pressure and temperature dependence of the rate coefficients, k(T, P), and time-resolved species profiles. Our theory showed excellent agreement with the measured rate coefficients. These are the first direct determination of the rate coefficients of the unimolecular decomposition of

关键词： 2-Methyl-1,3-dioxolane Absorption spectra High-temperature Pyrolysis RRKM-ME calculations Shock tube

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Opportunities in electrically tunable 2D materials beyond graphene: Recent progress and future outlook

arXiv

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arXiv 2021年

作者： Vincent, Tom Liang, Jiayun Singh, Simrjit Castanon, Eli G. Zhang, Xiaotian McCreary, Amber Jariwala, Deep Kazakova, Olga Al Balushi, Zakaria Y. Department of Quantum Technology National Physical Laboratory Hampton Road TeddingtonTW11 0LW United Kingdom Department of Materials Science and Engineering University of California BerkeleyCA94720 United States Department of Electrical and Systems Engineering University of Pennsylvania PhiladelphiaPA19104 United States Nanoscale Device Characterization Division Physical Measurement Laboratory National Institute of Standards and Technology GaithersburgMD20899 United States

The interest in two-dimensional and layered materials continues to expand, driven by the compelling properties of individual atomic layers that can be stacked and/or twisted into synthetic heterostructures. The plethora of electronic properties as well as the emergence of many different quasiparticles, including plasmons, polaritons, trions and excitons with large, tunable binding energies that all can be controlled and modulated through electrical means has given rise to many device applications. In addition, these materials exhibit both room-temperature spin and valley polarization, magnetism, superconductivity, piezoelectricity that are intricately dependent on the composition, crystal structure, stacking, twist angle, layer number and phases of these materials. Initial results on graphene exfoliated from single bulk crystals motivated the development of wide-area, high purity synthesis and heterojunctions with atomically clean interfaces. Now by opening this design space to new synthetic two-dimensional materials "beyond graphene", it is possible to explore uncharted opportunities in designing novel heterostructures for electrical tunable devices. To fully reveal the emerging functionalities and opportunities of these atomically thin materials in practical applications, this review highlights several representative and noteworthy research directions in the use of electrical means to tune these aforementioned physical and structural properties, with an emphasis on discussing major applications of beyond graphene 2D materials in tunable devices in the past few years and an outlook of what is to come in the next decade. © 2021, CC BY.

关键词： Graphene

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Cavity-mediated superthermal phonon correlations in the ultrastrong coupling regime

arXiv

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arXiv 2024年

作者： Kim, Dasom Hou, Jin Lee, Geon Agrawal, Ayush Kim, Sunghwan Zhang, Hao Bao, Di Baydin, Andrey Wu, Wenjing Tay, Fuyang Huang, Shengxi Chia, Elbert E.M. Kim, Dai-Sik Seo, Minah Mohite, Aditya D. Hagenmüller, David Kono, Junichiro Applied Physics Graduate Program Smalley–Curl Institute Rice University HoustonTX77005 United States Department of Electrical and Computer Engineering Rice University HoustonTX77005 United States Department of Materials Science and NanoEngineering Rice University HoustonTX77005 United States Sensor System Research Center Korea Institute of Science and Technology Seoul02792 Korea Republic of Department of Physics and Astronomy Seoul National University Seoul08826 Korea Republic of Department of Chemical and Biomolecular Engineering Rice University Houston77005 United States Ulsan44919 Korea Republic of Division of Physics and Applied Physics School of Physical and Mathematical Sciences Nanyang Technological University Singapore637371 Singapore Smalley–Curl Institute Rice University HoustonTX77005 United States Rice Advanced Materials Institute Rice University HoustonTX77005 United States KU–KIST Graduate School of Converging Science and Technology Korea University Seoul02841 Korea Republic of Université de Strasbourg CNRS Strasbourg67200 France Department of Physics and Astronomy Rice University HoustonTX77005 United States

Phonons, or vibrational quanta, are behind some of the most fundamental physical phenomena in solids, including superconductivity, Raman processes, and broken-symmetry phases. It is therefore of fundamental importance to find ways to harness phonons for controlling these phenomena and developing novel quantum technologies. However, the majority of current phonon control techniques rely on the use of intense external driving fields or strong anharmonicities, which restricts their range of applications. Here, we present a scheme for controlling the intensity fluctuations in phonon emission at room temperature based on multimode ultrastrong light–matter coupling. The multimode ultrastrong coupling regime is achieved by coupling two optical phonon modes in lead halide perovskites to an array of nanoslots, which operates as a single-mode cavity. The extremely small mode volume of the nanoslots enables unprecedented coupling strengths in a cavity phonon-polariton system. In the far-detuned, low-cavity-frequency regime, we demonstrate that the nanoslot resonator mediates an effective coupling between the phonon modes, resulting in superthermal phonon bunching in thermal equilibrium, both within the same mode and between different modes. Experimental results are in good agreement with a multimode Hopfield model. Our work paves the way for the tailoring of phonons to modify charge and energy transport in perovskite materials, with potential applications in light-collecting or emitting devices. Copyright © 2024, The Authors. All rights reserved.

关键词： Perovskite

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Cover Picture: Transforming Red Phosphorus Photocatalysis: Dual Roles of Pre-Anchored Ru Single Atoms in Defect and Interface engineering (Angew. Chem. Int. Ed. 45/2024)

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Angewandte Chemie International Edition 2024年第45期63卷

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Titelbild: Transforming Red Phosphorus Photocatalysis: Dual Roles of Pre-Anchored Ru Single Atoms in Defect and Interface engineering (Angew. Chem. 45/2024)

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Angewandte Chemie 2024年第45期136卷

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Semirealistic tight-binding model for Dzyaloshinskii-Moriya interaction

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physical Review B 2020年第22期102卷 224427-224427页

作者： Ahmed Hajr Abdulkarim Hariri Guilhem Manchon Sumit Ghosh Aurélien Manchon King Abdullah University of Science and Technology (KAUST) Physical Science and Engineering Division (PSE) Thuwal 23955-6900 Saudi Arabia Department of Physics King Fahd University of Petroleum and Minerals Dhahran 31261 Saudi Arabia King Abdullah University of Science and Technology (KAUST) Computer Electrical and Mathematical Science and Engineering Division (CEMSE) Thuwal 23955-6900 Saudi Arabia Aix-Marseille University CNRS CINaM Marseille France

In this work, we discuss the nature of Dzyaloshinskii-Moriya interaction (DMI) in transition metal heterostructures. We first derive the expression of DMI in the small-spatial-gradient limit using Keldysh formalism. This derivation provides us with a Green's function formula that is well adapted to tight-binding Hamiltonians. With this tool, we first uncover the role of orbital mixing: Using both a toy model and a realistic multiorbital Hamiltonian representing transition metal heterostructures, we show that symmetry breaking enables the onset of interfacial orbital momentum that is at the origin of the DMI. We then investigate the contribution of the different layers to the DMI and reveal that it can expand over several nonmagnetic metal layers depending on the Fermi energy, thereby revealing the complex orbital texture of the band structure. Finally, we examine the thickness dependence of DMI on both ferromagnetic and nonmagnetic metal thicknesses and we find that whereas the former remains very weak, the latter can be substantial.

关键词： Dzyaloshinskii-Moriya interaction Spin-orbit coupling Spintronics

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