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      A Nuclear Singlet Lifetime of More than One Hour in Room‐Temperature Solution†

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          Abstract

          Nuclear magnetic resonance (NMR) and magnetic resonance imaging (MRI) are supremely important techniques with numerous applications in almost all branches of science. However, until recently, NMR methodology was limited by the time constant T 1 for the decay of nuclear spin magnetization through contact with the thermal molecular environment. Long‐lived states, which are correlated quantum states of multiple nuclei, have decay time constants that may exceed T 1 by large factors. Here we demonstrate a nuclear long‐lived state comprising two 13C nuclei with a lifetime exceeding one hour in room‐temperature solution, which is around 50 times longer than T 1. This behavior is well‐predicted by a combination of quantum theory, molecular dynamics, and quantum chemistry. Such ultra‐long‐lived states are expected to be useful for the transport and application of nuclear hyperpolarization, which leads to NMR and MRI signals enhanced by up to five orders of magnitude.

          Translated abstract

          Lang lebe der Spin: Ein molekulares System basierend auf einem 13C 2‐markierten Naphthalin‐Kern wurde hergestellt, das in Lösung eine langlebige Singulett‐Kernspinordnung unterstützt. Ein Singulett‐Kernspin mit einer Lebensdauer von über einer Stunde konnte in Lösung bei Raumtemperatur beobachtet werden.

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          Beyond theT1Limit: Singlet Nuclear Spin States in Low Magnetic Fields

          Low-field nuclear spin singlet states may be used to store nuclear spin order in a room temperature liquid for a time much longer than the spin-lattice relaxation time constant T1. The low-field nuclear spin singlets are unaffected by intramolecular dipole-dipole relaxation, which is generally the predominant relaxation mechanism. We demonstrate storage of nuclear spin order for more than 10 times longer than the measured value of T1. This phenomenon may facilitate the development of nuclear spin hyperpolarization methods and may allow the study of motional processes which occur too slowly for existing NMR techniques. This is the first time that the memory of nuclear spins has been extended well beyond the T1 limit in a system lacking intrinsic magnetic equivalence.
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            Applications of dynamic nuclear polarization in 13C NMR in solids

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              The long-lived nuclear singlet state of 15N-nitrous oxide in solution.

              A 15N nuclear singlet lifetime of over 26 min has been observed in a solution of 15N2O, by using a field-cycling NMR pulse sequence. This observation suggests applications of hyperpolarized 15N2O in medical imaging and for flow and diffusion studies.
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                Author and article information

                Contributors
                g.pileio@soton.ac.uk
                mhl@soton.ac.uk
                Journal
                Angew Chem Weinheim Bergstr Ger
                Angew Chem Weinheim Bergstr Ger
                10.1002/(ISSN)1521-3757
                ANGE
                Angewandte Chemie (Weinheim an Der Bergstrasse, Germany)
                WILEY‐VCH Verlag (Weinheim )
                0044-8249
                1521-3757
                16 March 2015
                04 February 2015
                : 127
                : 12 ( doiID: 10.1002/ange.v127.12 )
                : 3811-3814
                Affiliations
                [ 1 ]School of Chemistry, University of Southampton, University Road, Southampton, SO17 1BJ (UK)
                Author notes
                [*] [* ]School of Chemistry, University of Southampton, University Road, Southampton, SO17 1BJ (UK)
                Article
                ANGE201411978
                10.1002/ange.201411978
                4955235
                27478258
                c3dcde64-8ca2-437c-8478-a90a2a4901e2
                © 2015 The Authors. Published by Wiley‐VCH Verlag GmbH & Co. KGaA. This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.

                Open access.

                History
                : 12 December 2014
                Page count
                Figures: 4, Tables: 1, References: 20, Pages: 4
                Funding
                Funded by: Funded Access
                Funded by: Engineering and Physical Sciences Research Council (UK)
                Funded by: European Research Council
                Funded by: Royal Society of Chemistry
                Funded by: Wolfson Foundation
                Categories
                Zuschrift
                Zuschriften
                NMR‐Spektroskopie
                Custom metadata
                2.0
                March 16, 2015
                Converter:WILEY_ML3GV2_TO_NLMPMC version:4.9.2 mode:remove_FC converted:20.07.2016

                langlebige spinzustände,kernspinrelaxation,nmr‐spektroskopie,singulettzustände

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