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Unraveling the Orbital Physics in a Canonical Orbital System KCuF3

Physical Review Letters 2021年第10期126卷 106401-106401页

作者： Jiemin Li Lei Xu Mirian Garcia-Fernandez Abhishek Nag H. C. Robarts A. C. Walters X. Liu Jianshi Zhou Krzysztof Wohlfeld Jeroen van den Brink Hong Ding Ke-Jin Zhou Diamond Light Source Harwell Campus Didcot OX11 0DE United Kingdom Beijing National Laboratory for Condensed Matter Physics and Institute of Physics Chinese Academy of Sciences Beijing 100190 China Institute for Theoretical Solid State Physics IFW Dresden Helmholtzstrasse 20 D-01069 Dresden Germany H. H. Wills Physics Laboratory University of Bristol Bristol BS8 1TL United Kingdom School of Physical Science and Technology ShanghaiTech University Shanghai 201210 China The Materials Science and Engineering Program Mechanical Engineering University of Texas at Austin Austin Texas 78712 USA Institute of Theoretical Physics Faculty of Physics University of Warsaw Pasteura 5 PL-02093 Warsaw Poland Institute for Theoretical Physics and Würzburg-Dresden Cluster of Excellence ct.qmat TU Dresden 01069 Dresden Germany

We explore the existence of the collective orbital excitations, orbitons, in the canonical orbital system KCuF3 using the Cu L3-edge resonant inelastic x-ray scattering. We show that the nondispersive high-energy peaks result from the Cu2+ dd orbital excitations. These high-energy modes display good agreement with the ab initio quantum chemistry calculation, indicating that the dd excitations are highly localized. At the same time, the low-energy excitations present clear dispersion. They match extremely well with the two-spinon continuum following the comparison with Müller ansatz calculations. The localized dd excitations and the observation of the strongly dispersive magnetic excitations suggest that the orbiton dispersion is below the resolution detection limit. Our results can reconcile with the strong local Jahn-Teller effect in KCuF3, which predominantly drives orbital ordering.

关键词： Orbital order Mott insulators Crystal-field theory Resonant inelastic x-ray scattering

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Irreparable Interphase Chemistry Degradation Induced by Temperature Pulse in Lithium-Ion Batteries

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Angewandte Chemie 2023年第50期135卷

作者： Dr. Zehao Cui Zezhou Guo Prof. Arumugam Manthiram Materials Science & Engineering Program and Texas Materials Institute The University of Texas at Austin Austin TX 78712 USA Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Investigation (equal) Methodology (lead) Validation (equal) Writing - original draft (lead) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Validation (equal) Writing - review & editing (supporting) Contribution: Conceptualization (supporting) Funding acquisition (lead) Methodology (supporting) Resources (lead) Supervision (lead) Validation (equal) Writing - review & editing (equal)

While it is widely recognized that the operating temperature significantly affects the energy density and cycle life of lithium-ion batteries, the consequence of electrode-electrolyte interphase chemistry to sudden environmental temperature changes remains inadequately understood. Here, we systematically investigate the effects of a temperature pulse (T pulse) on the electrochemical performance of LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) pouch full cells. By utilizing advanced characterization tools, such as time-of-flight secondary-ion mass spectrometry, we reveal that the T pulse can lead to an irreversible degradation of cathode-electrolyte interphase chemistry and architecture. Despite negligible immediate impacts on the solid-electrolyte interphase (SEI) on graphite anode, aggregated cathode-to-anode chemical crossover gradually degrades the SEI by catalyzing electrolyte reduction decomposition and inducing metallic dead Li formation because of insufficient cathode passivation after the T pulse. Consequently, pouch cells subjected to the T pulse show an inferior cycle stability to those free of the T pulse. This work unveils the effects of sudden temperature changes on the interphase chemistry and cell performance, emphasizing the importance of a proper temperature management in assessing performance.

关键词： Crossover Effects Electrode-Electrolyte Interphases Lithium-Ion Batteries NMC811 Temperature Pulse

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Solar Water Purification: High-Yield and Low-Cost Solar Water Purification via Hydrogel-Based Membrane Distillation (Adv. Funct. Mater. 19/2021)

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Advanced Functional materials 2021年第19期31卷

作者： Hengyi Lu Wen Shi Fei Zhao Wenjing Zhang Peixin Zhang Chenyang Zhao Guihua Yu College of Chemistry and Environmental Engineering Shenzhen University Shenzhen 518060 China Key Laboratory of Optoelectronic Devices and Systems of Ministry of Education and Guangdong Province College of Optoelectronic Engineering Shenzhen University Shenzhen 518060 China Materials Science and Engineering Program Texas Materials Institute The University of Texas at Austin Austin TX 78712 USA

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Bioinspired graphene-based silver nanoparticles: Fabrication, characterization and antibacterial activity

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materials Today: Proceedings 2020年 29卷 720-725页

作者： Ajay K. Potbhare Mayuri S. Umekar Prashant B. Chouke Mahendra B. Bagade S.K. Tarik Aziz Ahmed A. Abdala Ratiram G. Chaudhary Post Graduate Department of Chemistry Seth Kesarimal Porwal College of Arts Commerce and Science Kamptee 441001 India Department of Chemistry Bar Ilan Institute for Nanotechnology and Advanced Materials (BINA) Bar Ilan University Ramat-Gan 52900 Israel Chemical Engineering Program Texas A&M University at Qatar POB 23784 Doha Qatar

Herein we present a fabrication and antibacterial assays of novel silver nanoparticles (Ag NPs) on the surface of graphene oxide (GO) nanosheets as a multifunctional antibacterial material by using Pseudomonas aeruginosa biomass extract the nanocomposites has fabricated. as a synthesized material were characterized by spectroscopic technique including XRD, FTIR, EDX, Raman and TEM. XRD analysis specified the cubic crustal structure of NCs, while TEM rendered an average particle size of 25 nm of Ag-GO NCs. As a result, the fabricated Ag-GO NCs was tested against gram-positive and gram-negative strains and the results shows the Ag-GO NCs to be more effective against gram-negative bacteria ( *** ).

关键词： Graphene-based nanoparticles Ag-GO nanocomposites Pseudomonas aeruginosa Antibacterial activity

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Microscopic mechanism of van der Waals heteroepitaxy in the formation of MoS2/hBN vertical heterostructures

arXiv

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arXiv 2020年

作者： Okada, Mitsuhiro Maruyama, Mina Okada, Susumu Warner, Jamie H. Kureishi, Yusuke Uchiyama, Yosuke Taniguchi, Takashi Watanabe, Kenji Shimizu, Tetsuo Kubo, Toshitaka Shinohara, Hisanori Kitaura, Ryo Tsukuba Ibaraki305-8565 Japan Graduate School of Pure and Applied Sciences University of Tsukuba Tsukuba Ibaraki305-8571 Japan Walker Department of Mechanical Engineering University of Texas at Austin 204 East Dean Keeton Street AustinTX78712 United States Materials Graduate Program Texas Materials Institute University of Texas at Austin 204 East Dean Keeton Street AustinTX78712 United States Department of Chemistry Nagoya University Nagoya Aichi464-8602 Japan International Center for Materials Nanoarchitectonics National Institute for Materials Science Tsukuba Ibaraki305-0044 Japan Research Center for Functional Materials National Institute for Materials Science Tsukuba Ibaraki305-0044 Japan

Recent works have revealed that van der Waals (vdW) heteroepitaxial growth of 2D materials on crystalline substrates, such as hexagonal boron nitride (hBN), leads to formation of self-aligned grains, which results in defect-free stitching between the grains. However, how the weak vdW interaction causes strong limitation on crystal orientation of grains is still not understood yet. In this work, we have focused on investigation of microscopic mechanism of self-alignment of MoS2 grains in vdW epitaxial growth on hBN. Through calculation based on density functional theory and the Lennard-Jones potential, we found that interlayer energy between MoS2 and hBN strongly depends both on size and crystal orientation of MoS2. We also found that, when size of MoS2 is ca. 40 nm, rotational energy barrier can exceed ~ 1 eV, which should suppress rotation to align crystal orientation of MoS2 even at growth temperature. Copyright © 2020, The Authors. All rights reserved.

关键词： Van der Waals forces

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Tunneling spectroscopy of c-axis epitaxial cuprate junctions

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Physical Review B 2020年第22期101卷 224512-224512页

作者： Panpan Zhou Liyang Chen Ilya Sochnikov Tsz Chun Wu Matthew S. Foster Anthony T. Bollinger Xi He Ivan Božović Douglas Natelson Department of Physics and Astronomy Rice University Houston Texas 77005 USA Applied Physics Graduate Program Smalley-Curl Institute Rice University Houston Texas 77005 USA Department of Physics University of Connecticut Storrs Connecticut 06269 USA Brookhaven National Laboratory Upton New York 11973–5000 USA Department of Chemistry Yale University New Haven Connecticut 06520 USA Department of Electrical and Computer Engineering Rice University Houston Texas 77005 USA Department of Materials Science and NanoEngineering Rice University Houston Texas 77005 USA

Atomically precise epitaxial structures are unique systems for tunneling spectroscopy that minimize extrinsic effects of disorder. We present a systematic tunneling spectroscopy study, over a broad doping, temperature, and bias range, in epitaxial c-axis La2−xSrxCuO4/La2CuO4/La2−xSrxCuO4 heterostructures. The behavior of these superconductor/insulator/superconductor (SIS) devices is unusual. Down to 20 mK there is complete suppression of c-axis Josephson critical current with a barrier of only 2 nm of La2CuO4, and the zero-bias conductance remains at 20–30% of the normal-state conductance, implying a substantial population of in-gap states. Tunneling spectra show greatly suppressed coherence peaks. As the temperature is raised, the superconducting gap fills in rather than closing at Tc. For all doping levels, the spectra show an inelastic tunneling feature at ∼80 meV, suppressed as T exceeds Tc. These nominally simple epitaxial cuprate junctions deviate markedly from expectations based on the standard Bardeen-Cooper-Schrieffer theory.

关键词： Coherence length Impurities in superconductors Josephson effect Quasiparticles & collective excitations Superconducting gap Superconducting phase transition d-wave Cuprates Heterostructures High-temperature superconductors Multilayer thin films Scanning tunneling spectroscopy

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Optothermal nanolithography for versatile low-power patterning of atomic-thin two-dimensional materials

Optothermal nanolithography for versatile low-power patterni...

引用

CLEO: Applications and Technology, CLEO_AT 2018

作者： Li, Jingang Lin, Linhan Peng, Xiaolei Zheng, Yuebing Materials Science and Engineering Program and Texas Materials Institute The University of Texas at Austin AustinTX78712 United States Department of Mechanical Engineering The University of Texas at Austin AustinTX78712 United States

We report a new technique - optothermal nanolithography - to achieve fast, on-demand and arbitrary patterning of different atomic-thin two-dimensional materials using the highly localized plasmonic heating effect. ... 详细信息

ISBN: (纸本)9781943580422

关键词： Plasmonics

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Light programmable Micro/Nanomotors with Optically Tunable In-Phase Electric Polarization

arXiv

引用

arXiv 2019年

作者： Liang, Zexi Teal, Daniel Fan, Donglei Materials Science and Engineering Program University of Texas at Austin AustinTX78712 United States Department of Mechanical Engineering University of Texas at Austin AustinTX78712 United States

To develop active nanomaterials that can instantly respond to external stimuli with designed mechanical motions is an important step towards the realization of nanomachines and nanorobots. Herein, we present our finding of a versatile working mechanism that allows instantaneous change of alignment direction and speed of semiconductor nanowires in an external electric field with simple visible-light exposure. The light induced alignment switch can be cycled over hundreds of times and programmed to express words in Morse code. With theoretical analysis and numerical simulation, the working principle can be attributed to the optically tuned real-part (in-phase) electrical polarization of a semiconductor nanowire in an aqueous suspension. The manipulation principle is exploited to create a new type of microscale stepper motor that can readily switch between in-phase and out-phase modes, and agilely operate independent of neighboring motors with patterned light. This work could inspire the development of a new type of micro/nanomachines with individual and reconfigurable maneuverability for many applications. Copyright © 2019, The Authors. All rights reserved.

关键词： Stepping motors

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In situ Interweaved Binder Framework Mitigating the Structural and Interphasial Degradations of High-nickel Cathodes in Lithium-ion Batteries

引用

Angewandte Chemie 2023年第15期135卷

作者： Dr. Biyu Jin Zehao Cui Prof. Arumugam Manthiram Materials Science and Engineering Program and Texas Materials Institute The University of Texas at Austin Austin TX 78712 USA Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (equal) Writing - original draft (lead) Contribution: Conceptualization (supporting) Data curation (equal) Formal analysis (supporting) Investigation (supporting) Methodology (equal) Writing - review & editing (equal) Contribution: Conceptualization (equal) Funding acquisition (lead) Investigation (supporting) Project administration (lead) Resources (lead) Supervision (lead) Validation (equal) Writing - review & editing (equal)

The practical viability of high-nickel layered oxide cathodes is compromised by the interphasial and structural degradations. Herein, we demonstrate that by applying an in situ interweaved binder, the cycling stability of high-nickel cathodes can be significantly improved. Specifically, the results show that the resilient binder network immobilizes the transition-metal ions, suppresses electrolyte oxidative decomposition, and mitigates cathode particles pulverization, thus resulting in suppressed cathode-to-anode chemical crossover and ameliorated chemistry and architecture of electrode-electrolyte interphases. Pouch full cells with high-mass-loading LiNi 0.8 Mn 0.1 Co 0.1 O 2 cathodes achieve 0.02 % capacity decay per cycle at 1 C rate over 1 000 deep cycles at 4.4 V (vs. graphite). This work demonstrates a rational structural and compositional design strategy of polymer binders to mitigate the structural and interphasial degradations of high-Ni cathodes in lithium-ion batteries.

关键词： Cathode-to-Anode Crossover Electrode-Electrolyte Interphase High-Nickel Cathode In Situ Interweaved Binder Particles Pulverization

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Highly Elastic Interconnected Porous Hydrogels through Self-Assembled Templating for Solar Water Purification

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Angewandte Chemie 2021年第3期134卷

作者： Youhong Guo Dr. Luize Scalco de Vasconcelos Dr. Neha Manohar Dr. Jiafeng Geng Prof. Keith P. Johnston Prof. Guihua Yu Materials Science and Engineering Program and Walker Department of Mechanical Engineering The University of Texas at Austin Austin TX 78712 USA Department of Aerospace Engineering and Engineering Mechanics The University of Texas at Austin Austin TX 78712 USA McKetta Department of Chemical Engineering The University of Texas at Austin Austin TX 78712 USA Department of Chemical Engineering Chang'an University Xi'an Shannxi 710061 China

Interfacial evaporation using porous hydrogels has demonstrated highly effective solar evaporation performance under natural sunlight to ensure an affordable clean water supply. However, it remains challenging to realize scalable and ready-to-use hydrogel materials with durable mechanical properties. Here, self-assembled templating (SAT) is developed as a simple yet effective method to fabricate large-scale elastic hydrogel evaporators with excellent desalination performance. The highly interconnected porous structure of the hydrogels with low tortuosity and tunable pore size enables high level of tunability on the water transport rate. With superior elasticity, the porous hydrogels are easy to process with a rapid shape recovery after being rolled, folded, and twisted over hundred times, and exhibit highly effective and stable evaporation with an evaporation rate of ≈2.8 kg m −2 h −1 and ≈90 % solar-to-vapor efficiency. It is anticipated that this SAT strategy, without the typical need for freeze-drying, will accelerate the industrialization of hydrogel solar evaporators for practical applications.

关键词： elasticity interconnectivity porous hydrogels solar water purification template synthesis

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