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      Room-temperature quantum coherence of entangled multiexcitons in a metal-organic framework

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          Abstract

          Singlet fission can generate an exchange-coupled quintet triplet pair state 5TT, which could lead to the realization of quantum computing and quantum sensing using entangled multiple qubits even at room temperature. However, the observation of the quantum coherence of 5TT has been limited to cryogenic temperatures, and the fundamental question is what kind of material design will enable its room-temperature quantum coherence. Here, we show that the quantum coherence of singlet fission–derived 5TT in a chromophore-integrated metal-organic framework can be over hundred nanoseconds at room temperature. The suppressed motion of the chromophores in ordered domains within the metal-organic framework leads to the enough fluctuation of the exchange interaction necessary for 5TT generation but, at the same time, does not cause severe 5TT decoherence. Furthermore, the phase and amplitude of quantum beating depend on the molecular motion, opening the way to room-temperature molecular quantum computing based on multiple quantum gate control.

          Abstract

          Room-temperature quantum coherence of entangled multiexcitons is realized by suppressed chromophore motion.

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          Most cited references53

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          Functional Porous Coordination Polymers

          The chemistry of the coordination polymers has in recent years advanced extensively, affording various architectures, which are constructed from a variety of molecular building blocks with different interactions between them. The next challenge is the chemical and physical functionalization of these architectures, through the porous properties of the frameworks. This review concentrates on three aspects of coordination polymers: 1). the use of crystal engineering to construct porous frameworks from connectors and linkers ("nanospace engineering"), 2). characterizing and cataloging the porous properties by functions for storage, exchange, separation, etc., and 3). the next generation of porous functions based on dynamic crystal transformations caused by guest molecules or physical stimuli. Our aim is to present the state of the art chemistry and physics of and in the micropores of porous coordination polymers.
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            Quantum supremacy using a programmable superconducting processor

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              A new zirconium inorganic building brick forming metal organic frameworks with exceptional stability.

              Porous crystals are strategic materials with industrial applications within petrochemistry, catalysis, gas storage, and selective separation. Their unique properties are based on the molecular-scale porous character. However, a principal limitation of zeolites and similar oxide-based materials is the relatively small size of the pores, typically in the range of medium-sized molecules, limiting their use in pharmaceutical and fine chemical applications. Metal organic frameworks (MOFs) provided a breakthrough in this respect. New MOFs appear at a high and an increasing pace, but the appearances of new, stable inorganic building bricks are rare. Here we present a new zirconium-based inorganic building brick that allows the synthesis of very high surface area MOFs with unprecedented stability. The high stability is based on the combination of strong Zr-O bonds and the ability of the inner Zr6-cluster to rearrange reversibly upon removal or addition of mu3-OH groups, without any changes in the connecting carboxylates. The weak thermal, chemical, and mechanical stability of most MOFs is probably the most important property that limits their use in large scale industrial applications. The Zr-MOFs presented in this work have the toughness needed for industrial applications; decomposition temperature above 500 degrees C and resistance to most chemicals, and they remain crystalline even after exposure to 10 tons/cm2 of external pressure.
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                Author and article information

                Contributors
                Role: ConceptualizationRole: Data curationRole: Formal analysisRole: Funding acquisitionRole: InvestigationRole: VisualizationRole: Writing - original draftRole: Writing - review & editing
                Role: ConceptualizationRole: InvestigationRole: MethodologyRole: ResourcesRole: ValidationRole: Writing - original draft
                Role: Data curationRole: InvestigationRole: VisualizationRole: Writing - original draftRole: Writing - review & editing
                Role: ConceptualizationRole: MethodologyRole: Resources
                Role: ConceptualizationRole: Funding acquisitionRole: ResourcesRole: SupervisionRole: ValidationRole: VisualizationRole: Writing - review & editing
                Role: Formal analysisRole: Funding acquisitionRole: InvestigationRole: ResourcesRole: Validation
                Role: Formal analysisRole: InvestigationRole: Resources
                Role: Resources
                Role: Formal analysisRole: SoftwareRole: Visualization
                Role: Formal analysisRole: InvestigationRole: Resources
                Role: ConceptualizationRole: Data curationRole: Formal analysisRole: Funding acquisitionRole: InvestigationRole: MethodologyRole: Project administrationRole: ResourcesRole: SoftwareRole: SupervisionRole: ValidationRole: VisualizationRole: Writing - original draftRole: Writing - review & editing
                Role: ConceptualizationRole: Data curationRole: Formal analysisRole: Funding acquisitionRole: InvestigationRole: MethodologyRole: Project administrationRole: ResourcesRole: SoftwareRole: SupervisionRole: ValidationRole: VisualizationRole: Writing - original draftRole: Writing - review & editing
                Role: ConceptualizationRole: Data curationRole: Funding acquisitionRole: Project administrationRole: ResourcesRole: SupervisionRole: ValidationRole: VisualizationRole: Writing - original draft
                Journal
                Sci Adv
                Sci Adv
                sciadv
                advances
                Science Advances
                American Association for the Advancement of Science
                2375-2548
                05 January 2024
                03 January 2024
                : 10
                : 1
                : eadi3147
                Affiliations
                [ 1 ]Department of Applied Chemistry, Graduate School of Engineering, Kyushu University, 744 Moto-oka, Nishi-ku, Fukuoka 819-0395, Japan.
                [ 2 ]Molecular Photoscience Research Center, Kobe University, 1-1, Rokkodai-cho, Nada-ku, Kobe 657-8501, Japan.
                [ 3 ]CREST, JST, Honcho 4-1-8, Kawaguchi, Saitama 332-0012, Japan.
                [ 4 ]RIKEN, RIKEN Center for Emergent Matter Science, Wako, Saitama 351-0198, Japan.
                [ 5 ]Center for Molecular Systems (CMS), Kyushu University, 744 Moto-oka, Nishi-ku, Fukuoka 819-0395, Japan.
                [ 6 ]Department of Chemistry, Graduate School of Science, Kyushu University, 744 Moto-oka, Nishi-ku, Fukuoka 819-0395, Japan.
                [ 7 ]Department of Chemistry, Graduate School of Science, Kobe University, 1-1, Rokkodai-cho, Nada-ku, Kobe 657-8501, Japan.
                [ 8 ]Graduate School of Human Development and Environment, Kobe University, 3-11 Tsurukabuto, Nada, Kobe 657-8501, Japan.
                [ 9 ]FOREST, JST, Honcho 4-1-8, Kawaguchi, Saitama 332-0012, Japan.
                Author notes
                [†]

                These authors contributed equally to this work.

                Author information
                https://orcid.org/0009-0006-2340-5790
                https://orcid.org/0009-0006-2604-9023
                https://orcid.org/0000-0002-8779-5250
                https://orcid.org/0000-0002-4147-6713
                https://orcid.org/0000-0001-8527-151X
                https://orcid.org/0000-0002-7695-2644
                https://orcid.org/0000-0003-1724-2009
                https://orcid.org/0009-0005-3574-483X
                https://orcid.org/0000-0002-9207-8424
                https://orcid.org/0000-0001-8370-9362
                https://orcid.org/0000-0001-6748-1337
                https://orcid.org/0000-0003-0297-6544
                Article
                adi3147
                10.1126/sciadv.adi3147
                10775993
                38170775
                31c85f3b-efb0-4f42-9cf9-36f32ba078db
                Copyright © 2024 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).

                This is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license, which permits use, distribution, and reproduction in any medium, so long as the resultant use is not for commercial advantage and provided the original work is properly cited.

                History
                : 19 April 2023
                : 28 November 2023
                Funding
                Funded by: FundRef http://dx.doi.org/10.13039/100008608, Sumitomo Foundation;
                Funded by: FundRef http://dx.doi.org/10.13039/501100001691, Japan Society for the Promotion of Science;
                Award ID: JP20H05676
                Funded by: FundRef http://dx.doi.org/10.13039/501100001691, Japan Society for the Promotion of Science;
                Award ID: JP23KJ1694
                Funded by: FundRef http://dx.doi.org/10.13039/501100001691, Japan Society for the Promotion of Science;
                Award ID: JP20H02713, JP22K19051
                Funded by: FundRef http://dx.doi.org/10.13039/501100001691, Japan Society for the Promotion of Science;
                Award ID: JP20K21174, JP20KK0120, JP22K19008, JP20H05832
                Funded by: FundRef http://dx.doi.org/10.13039/501100002241, Japan Science and Technology Agency;
                Award ID: JPMJFR201Y
                Funded by: FundRef http://dx.doi.org/10.13039/501100002241, Japan Science and Technology Agency;
                Award ID: JPMJSP2136
                Funded by: FundRef http://dx.doi.org/10.13039/501100002241, Japan Science and Technology Agency;
                Award ID: JPMJFS2132
                Funded by: FundRef http://dx.doi.org/10.13039/501100008662, Murata Science Foundation;
                Funded by: FundRef http://dx.doi.org/10.13039/501100012018, Research Foundation for Opto-Science and Technology;
                Funded by: FundRef http://dx.doi.org/10.13039/501100002241, Japan Science and Technology Agency;
                Award ID: JPMJCR23I6
                Funded by: FundRef http://dx.doi.org/10.13039/501100012018, Research Foundation for Opto-Science and Technology;
                Funded by: Kyushu University Platform of Inter-/Transdisciplinary Energy Research (Q-PIT);
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                Materials Science
                Physical Sciences
                Materials Science
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                Jeanelle Ebreo

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