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Diversification of the Carbodicarbene Class by Embedding an Anionic Component in its Scaffold

Chemistry - A European Journal 2023年第71期29卷 e202302886页

作者： Yu, Cheng-Han Au-Yeung, Ka-Chun Liu, Ruiqin Lee, Chao-Hsien Jiang, Dandan Semagne Aweke, Bamlaku Wu, Chia-Hung Wang, Yu-Jou Wang, Ting-Hsuan Voon Kong, Kien Yap, Glenn P. A. Chen, Wen-Ching Frenking, Gernot Zhao, Lili Ong, Tiow-Gan Institute of chemistry Academia Sinica Taipei115201 Taiwan School of Chemistry and Molecular Engineering State Key Laboratory of Materials-Oriented Chemical Engineering Nanjing Tech University Nanjing China Fachbereich Chemie Philipps-Universität Marburg Hans-Meerwein-Strasse MarburgD-35043 Germany Department of Chemistry and Biochemistry University of Delaware NewarkDE United States Department of Chemistry National Taiwan University Taipei Taiwan Department of Applied Chemistry National Yang Ming Chiao Tung University Hsinchu Taiwan Sustainable Chemical Science and Technology Taiwan International Graduate Program Academia Sinica Taipei Taiwan Corporate R&D Center LCY Chemical Corporation Kaohsiung Taiwan Department of Medicinal and Applied Chemistry Kaohsiung Medical University Kaohsiung Taiwan

Carbodicarbene (CDC) has become an emerging ligand in many fields due to its strong σ-donating ability. 2- moiety within the framework to leverage the electronic feature of carbon carbone. The elucidation of X-ray crystal structures, ligand competition as well as transmetallation experiments suggest that the anionic moiety has enhanced the overall donor strength of the traditional neutral CDC. Importantly, this anionic scaffold exhibits a facile second coordination toward Au(I), Ag(I) and Pd(II) without any external ligand assistance, whereas previously reported neutral pincer CDC complexes do not possess a two-fold donor capacity. The analysis of the bonding situation via theoretical methods shows that the description of the anionic CDC moieties in terms of dative bonding is preferred over the model of delocalized positive charge, as it accounts for the two-fold donor ability of the divalent carbon atom, preserving a characteristic feature of a carbone. © 2023 Wiley-VCH GmbH.

关键词： Scaffolds

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Bispropylurea bridged polysilsesquioxane: A microporous MOF-like material for molecular recognition

arXiv

引用

arXiv 2021年

作者： Doustkhah, Esmail Tahawy, Rafat Simon, Ulla Tsunoji, Nao Ide, Yusuke Hanaor, Dorian A.H. Hussein N. Assadi, M. 1-1 Namiki Tsukuba Ibaraki305-0044 Japan Fachgebiet Keramische Werkstoffe Technische Universität Berlin Berlin10623 Germany Graduate School of Advanced Science and Engineering Applied Chemistry Program Hiroshima University 1-4-1 Kagamiyama Higashi-Hiroshima739-8527 Japan School of Materials Science and Engineering The University of New South Wales SydneyNSW2052 Australia

Microporous organosilicas assembled from polysilsesquioxane (POSS) building blocks are promising materials that are yet to be explored in-depth. Here, we investigate the processing and molecular structure of bispropylurea bridged POSS (POSS-urea), synthesised through the acidic condensation of 1,3-bis(3-(triethoxysilyl)propyl)urea (BTPU). Experimentally, we show that POSS-urea has excellent functionality for molecular recognition toward acetonitrile with an adsorption level of 74 mmol/g, which compares favourably to MOFs and zeolites, with applications in volatile organic compounds (VOC). The acetonitrile adsorption capacity was 132-fold higher relative to adsorption capacity for toluene, which shows the pores are highly selective towards acetonitrile adsorption due to their size and arrangement. Theoretically, our tight-binding density functional and molecular dynamics calculations demonstrated that this BTPU based POSS is microporous with an irregular placement of the pores. Structural studies confirm maximal pore sizes of ~ 1 nm, with POSS cages possessing an approximate edge length of ~ 3.16 Å. © 2021, CC BY.

关键词： Urea

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Identifying topologically associating domains using differential kernels

arXiv

引用

arXiv 2023年

作者： Maisuradze, Luka King, Megan C. Surovtsev, Ivan V. Mochrie, Simon G.J. Shattuck, Mark D. O’Hern, Corey S. Department of Molecular Biophysics and Biochemistry Yale University New HavenCT United States Department of Cell Biology Yale School of Medicine New HavenCT United States Department of Physics Yale University New HavenCT United States Benjamin Levich Institute Physics Department The City College of New York New YorkNY United States Department of Mechanical Engineering and Materials Science Yale University New HavenCT United States Graduate Program in Computational Biology and Bioinformatics Yale University New HavenCT United States

Chromatin is a polymer complex of DNA and proteins that regulates gene expression. The three-dimensional (3D) structure and organization of chromatin controls DNA transcription and replication. High-throughput chromatin conformation capture techniques generate Hi-C maps that can provide insight into the 3D structure of chromatin. Hi-C maps can be represented as a symmetric matrix Aij, where each element represents the average contact probability or number of contacts between chromatin loci i and j. Previous studies have detected topologically associating domains (TADs), or self-interacting regions in Aij within which the contact probability is greater than that outside the region. Many algorithms have been developed to identify TADs within Hi-C maps. However, most TAD identification algorithms are unable to identify nested or overlapping TADs and for a given Hi-C map there is significant variation in the location and number of TADs identified by different methods. We develop a novel method to identify TADs, KerTAD, using a kernel-based technique from computer vision and image processing that is able to accurately identify nested and overlapping TADs. We benchmark this method against state-of-the-art TAD identification methods on both synthetic and experimental data sets. We find that the new method consistently has higher true positive rates (TPR) and lower false discovery rates (FDR) than all tested methods for both synthetic and manually annotated experimental Hi-C maps. The TPR for KerTAD is also largely insensitive to increasing noise and sparsity, in contrast to the other methods. We also find that KerTAD is consistent in the number and size of TADs identified across replicate experimental Hi-C maps for several organisms. Thus, KerTAD will improve automated TAD identification and enable researchers to better correlate changes in TADs to biological phenomena, such as enhancer-promoter interactions and disease states. © 2023, CC BY.

关键词： Topology

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High-performance Removal of Anti-inflammatory Using Activated Carbon from Water Treatment Plant Sludge: Fixed-bed and Batch Studies

Research Square

引用

Research Square 2021年

作者： Filho, Alaor Valério Tholozan, Luana Vaz Arim, Aline Lemos de Almeida, André Ricardo Felkl da Rosa, Gabriela Silveira Graduate Program in Science and Engineering of Materials Federal University of Pampa 1650 Maria Anunciação Gomes Godoy Avenue Rio Grande do Sul Bagé96413-172 Brazil Chemical Engineering Federal University of Pampa 1650 Maria Anunciação Gomes Godoy Avenue Rio Grande do Sul Bagé96413-172 Brazil

Activated carbon from water treatment sludge (WASC) was employed as adsorbent material to remove the anti-inflammatory Nimesulide (NM) from aqueous solutions. NM adsorption was performed in batch and fixed-bed systems, evaluating pH, adsorbent dosage, adsorption kinetics, equilibrium isotherm, continuous adsorption, and simulated effluents. The kinetic data were best fitted to the Elovich model and Intraparticle diffusion reaching the equilibrium at 120 min. Langmuir model presented a better description of the equilibrium data with the maximum adsorption capacity (qmax) of 274.99 mg g-1 from NM adsorption by WASC. The adsorbent was tested in two simulated hospital effluents and proved to be an excellent adsorbent for removing NM from an aqueous solution with the presence of salts, sugars, and other inorganics. Finally, WASC was applied in fixed-bed NM adsorption obtaining the adsorption capacity of 217.28 mg g-1 © 2021, CC BY.

关键词： Adsorption

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Deformed Fredkin model for the ν=5/2 Moore-Read state on thin cylinders

arXiv

引用

arXiv 2023年

作者： Voinea, Cristian Pu, Songyang Kirmani, Ammar Ghaemi, Pouyan Rahmani, Armin Papić, Zlatko School of Physics and Astronomy University of Leeds LeedsLS2 9JT United Kingdom Theoretical Division T-4 Los Alamos National Laboratory Los AlamosNM87545 United States Physics Department City College of the City University of New York NY10031 United States Physics Program Graduate Center of City University of New York NY10031 United States Department of Physics and Astronomy Advanced Materials Science and Engineering Center Western Washington University BellinghamWA98225 United States

We propose a frustration-free model for the Moore-Read quantum Hall state on sufficiently thin cylinders with circumferences 7 magnetic lengths. While the Moore-Read Hamiltonian involves complicated long-range interactions between triplets of electrons in a Landau level, our effective model is a simpler one-dimensional chain of qubits with deformed Fredkin gates. We show that the ground state of the Fredkin model has high overlap with the Moore-Read wave function and accurately reproduces the latter’s entanglement properties. Moreover, we demonstrate that the model captures the dynamical response of the Moore-Read state to a geometric quench, induced by suddenly changing the anisotropy of the system. We elucidate the underlying mechanism of the quench dynamics and show that it coincides with the linearized bimetric field theory. The minimal model introduced here can be directly implemented as a first step towards quantum simulation of the Moore-Read state, as we demonstrate by deriving an efficient circuit approximation to the ground state and implementing it on IBM quantum processor. © 2023, CC BY.

关键词： Ground state

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Al2O3-CaO macroporous ceramics containing hydrocalumite-like phases

arXiv

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arXiv 2020年

作者： Borges, O.H. Santos, T. Salvini, V.R. Pandolfelli, V.C. Federal University of São Carlos Graduate Program in Materials Science and Engineering Rua Jordão Borghetti 480 Sertãozinho SP14160-050 Brazil

A mechanism to explain the lower onset strengthening temperature induced by CaCO3 in alumina-based macroporous ceramics is proposed, which relies on hydrocalumite-like phase formation during processing. Close to 600 °C, such phases are decomposed to lime and mayenite (12CaO·7Al2O3), where the latter, due to its intrinsic nanoporosity and high thermal reactivity, generates bonds between the ceramic particles at ~700ºC, resulting in microstructure strengthening. Based on this premise, the authors concluded that other Ca2+ sources could act similarly. Indeed, compositions containing Ca(OH)2 or CaO showed the same effect on the onset strengthening temperature, which reinforces the proposed mechanism. The results attained indicated that macroporous insulators could be thermally treated at lower temperatures, just to acquire enough mechanical strength for installation, finishing in-situ their firing process. Besides that, lower sintering temperatures could be used to produce macroporous ceramics that would be applied in low thermal demand environments, e.g. aluminum industries. Copyright © 2020, The Authors. All rights reserved.

关键词： Sintering

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Ultrastrong Spin-Photon Coupling in Gadolinium Gallium Garnet

Ultrastrong Spin-Photon Coupling in Gadolinium Gallium Garne...

引用

Conference on Lasers and Electro-Optics (CLEO)

作者： T. Elijah Kritzell Junzhe Bao Jacques Doumani Jae Joon Lee Hongjing Xu Fuyang Tay Hiroyuki Nojiri Motoaki Bamba Andrey Baydin Junichiro Kono Department of Electrical and Computer Engineering Rice University Houston Texas USA Applied Physics Graduate Program Smalley-Curl Institute Rice University Houston Texas USA Department of Physics and Astronomy Rice University Houston Texas USA Institute for Materials Research Tohoku University Senai Japan The Hakubi Center for Advanced Research Kyoto University Kyoto Japan Department of Physics I Kyoto University Kyoto Japan Smalley-Curl Institute Rice University Houston Texas USA Department of Material Science and NanoEngineering Rice University Houston Texas USA

We examine ultrastrong coupling of an ensemble of paramagnetic spins in Gd 3 Ga 5 O 12 with terahertz photons in the presence of a high external magnetic field both in the bulk and thin-film limits.

ISBN: (纸本)9781957171258

We examine ultrastrong coupling of an ensemble of paramagnetic spins in Gd 3 Ga 5 O 12 with terahertz photons in the presence of a high external magnetic field both in the bulk and thin-film limits.

关键词： CCD cameras Condensed matter Magnetic fields Photons Quantum optics Terahertz spectroscopy

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Graphene Terahertz Devices for Sensing and Communication

arXiv

引用

arXiv 2024年

作者： Samaha, Anna-Christina Doumani, Jacques Kritzell, T. Elijah Xu, Hongjing Baydin, Andrey Ajayan, Pulickel M. Tahchi, Mario El Kono, Junichiro Laboratory of Biomaterials and Intelligent Materials Department of Physics Faculty of Sciences 2 Lebanese University P.O. Box 90656 Jdeidet Lebanon Department of Electrical and Computer Engineering Rice University 6100 Main Street HoustonTX77005 United States Applied Physics Graduate Program Smalley–Curl Institute Rice University 6100 Main Street HoustonTX77005 United States Department of Physics and Astronomy Rice University 6100 Main Street HoustonTX77005 United States Smalley–Curl Institute Rice University 6100 Main Street HoustonTX77005 United States Department of Materials Science and NanoEngineering Rice University 6100 Main Street HoustonTX77005 United States Carbon Hub Rice University 6100 Main Street HoustonTX77005 United States

Graphene-based terahertz (THz) devices have emerged as promising platforms for a variety of applications, leveraging graphene’s unique optoelectronic properties. This review explores recent advancements in utilizing graphene in THz technology, focusing on two main aspects: THz molecular sensing and THz wave modulation. In molecular sensing, the environment-sensitive THz transmission and emission properties of graphene are utilized for enabling molecular adsorption detection and biomolecular sensing. This capability holds significant potential, from the detection of pesticides to DNA at high sensitivity and selectivity. In THz wave modulation, crucial for next-generation wireless communication systems, graphene demonstrates remarkable potential in absorption modulation when gated. Novel device structures, spectroscopic systems, and metasurface architectures have enabled enhanced absorption and wave modulation. Furthermore, techniques such as spatial phase modulation and polarization manipulation have been explored. From sensing to communication, graphene-based THz devices present a wide array of opportunities for future research and development. Finally, advancements in sensing techniques not only enhance biomolecular analysis but also contribute to optimizing graphene’s properties for communication by enabling efficient modulation of electromagnetic waves. Conversely, developments in communication strategies inform and enhance sensing capabilities, establishing a mutually beneficial relationship. © 2024, CC BY.

关键词： Graphene

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Frontispiece: Visible-Light-Driven Solid-State Fluorescent Photoswitches for High-Level Information Encryption

引用

Angewandte Chemie International Edition 2024年第51期63卷

作者： Zhiyuan Han Prof. Meixia He Prof. Gang Wang Prof. Jean-Marie Lehn Prof. Quan Li Institute of Advanced Materials and School of Chemistry and Chemical Engineering Southeast University Nanjing 211189 China School of Chemical Engineering Xi'an University Xi'an 710065 China Laboratoire de Chimie Supramoléculaire Institut de Science et d'Ingénierie Supramoléculaires (lSlS) Université de Strasbourg 8 allée Gaspard Monge Strasbourg 67000 France Materials Science Graduate Program Kent State University Kent OH 44242 USA

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Multimode Ultrastrong Coupling in Three-Dimensional Photonic-Crystal Cavities

arXiv

引用

arXiv 2023年

作者： Tay, Fuyang Mojibpour, Ali Sanders, Stephen Liang, Shuang Xu, Hongjing Gardner, Geoff C. Baydin, Andrey Manfra, Michael J. Alabastri, Alessandro Hagenmüller, David Kono, Junichiro Department of Electrical and Computer Engineering Rice University HoustonTX77005 United States Applied Physics Graduate Program Smalley–Curl Institute Rice University HoustonTX77005 United States Department of Physics and Astronomy Purdue University West LafayetteIN47907 United States Birck Nanotechnology Center Purdue University West LafayetteIN47907 United States Department of Physics and Astronomy Rice University HoustonTX77005 United States School of Electrical and Computer Engineering Purdue University West LafayetteIN47907 United States Smalley–Curl Institute Rice University HoustonTX77005 United States School of Materials Engineering Purdue University West LafayetteIN47907 United States Université de Strasbourg CNRS Strasbourg67000 France Department of Materials Science and NanoEngineering Rice University HoustonTX77005 United States

Recent theoretical studies have highlighted the role of spatially varying cavity electromagnetic fields in exploring novel cavity quantum electrodynamics (cQED) phenomena, such as the potential realization of the elusive Dicke superradiant phase transition. One-dimensional photonic-crystal cavities (PCCs), widely used for studying solid-state cQED systems, have uniform spatial profiles in the lateral plane. Three-dimensional (3D) PCCs, which exhibit discrete in-plane translational symmetry, overcome this limitation, but fabrication challenges have hindered the achievement of strong coupling in 3D-PCCs. Here, we report the realization of multimode ultrastrong coupling in a 3D-PCC at terahertz frequencies. The multimode coupling between the 3D-PCC’s cavity modes and the cyclotron resonance of a Landau-quantized two-dimensional electron gas in GaAs is significantly influenced by the spatial profiles of the cavity modes, leading to distinct coupling scenarios depending on the probe polarization. Our experimental results are in excellent agreement with a multimode extended Hopfield model that accounts for the spatial inhomogeneity of the cavity field. Guided by the model, we discuss the possible strong ground-state correlations between different cavity modes and introduce relevant figures of merit for the multimode ultrastrong coupling regime. Our findings emphasize the importance of spatially nonuniform cavity mode profiles in probing nonintuitive quantum phenomena expected for the ground states of cQED systems in the ultrastrong coupling regime. Copyright © 2023, The Authors. All rights reserved.

关键词： Electron cyclotron resonance

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