Mixed-valence compounds as polarizing agents for Overhauser dynamic nuclear polarization in solids

Andrei Gurinov; Sieland Benedikt; Andrey Kuzhelev; Hossam Elgabarty; Thomas D Kühne; Thomas Prisner; Jan Paradies; Marc Baldus; Konstantin L Ivanov; Svetlana Pylaeva

doi:10.1002/anie.202103215

Mixed-valence compounds as polarizing agents for Overhauser dynamic nuclear polarization in solids

Andrei Gurinov, Sieland Benedikt, Andrey Kuzhelev, Hossam Elgabarty, Thomas D Kühne, Thomas Prisner, Jan Paradies, Marc Baldus, Konstantin L Ivanov, Svetlana Pylaeva

Research output: Contribution to journal › Article › Academic › peer-review

Abstract

Herein, we investigate a novel set of polarizing agents—mixed-valence compounds—by theoretical and experimental methods and demonstrate their performance in high-field dynamic nuclear polarization (DNP) NMR experiments in the solid state. Mixed-valence compounds constitute a group of molecules in which molecular mobility persists even in solids. Consequently, such polarizing agents can be used to perform Overhauser-DNP experiments in the solid state, with favorable conditions for dynamic nuclear polarization formation at ultra-high magnetic fields.

Original language	English
Pages (from-to)	15371-15375
Number of pages	5
Journal	Angewandte Chemie-International Edition
Volume	60
Issue number	28
Early online date	28 Apr 2021
DOIs	https://doi.org/10.1002/anie.202103215
Publication status	Published - 5 Jul 2021

Bibliographical note

Funding Information:
This work has been supported by iNEXT-Discovery, grant number 871037, funded by the Horizon 2020 program of the European Commission. Svetlana Pylaeva would like to thank Prof. Matvey Fedin, Dr. Yury Lebedev for fruitful discussions of EPR experiments and organic synthesis. HE acknowledges the DFG for funding his temporary position as a principal investigator (Eigene Stelle). TDK acknowledges funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (grant agreement no. 716142). The generous allocation of supercomputer time by the Paderborn Center for Parallel Computing (PC2) is kindly acknowledged. JP acknowledges the DFG for funding (PA1562-14/1). The DNP experiments were supported by the Dutch Research Council (NWO grants 700.11.344 and 700.58.102 to MB). Open access funding enabled and organized by Projekt DEAL.

Funding Information:
This work has been supported by iNEXT‐Discovery, grant number 871037, funded by the Horizon 2020 program of the European Commission. Svetlana Pylaeva would like to thank Prof. Matvey Fedin, Dr. Yury Lebedev for fruitful discussions of EPR experiments and organic synthesis. HE acknowledges the DFG for funding his temporary position as a principal investigator (Eigene Stelle). TDK acknowledges funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (grant agreement no. 716142). The generous allocation of supercomputer time by the Paderborn Center for Parallel Computing (PC2) is kindly acknowledged. JP acknowledges the DFG for funding (PA1562‐14/1). The DNP experiments were supported by the Dutch Research Council (NWO grants 700.11.344 and 700.58.102 to MB). Open access funding enabled and organized by Projekt DEAL.

Publisher Copyright:
© 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH

Keywords

DNP in solids
Overhauser effect
ab initio calculations
mixed valence compounds
molecular dynamics

Access to Document

10.1002/anie.202103215Licence: CC BY

Angew Chem Int Ed - 2021 - Gurinov - Mixed‐Valence Compounds as Polarizing Agents for Overhauser Dynamic NuclearFinal published version, 0.98 MBLicence: CC BY

Cite this

@article{0ba48a111c6348eb9a2a6bde46b867c6,

title = "Mixed-valence compounds as polarizing agents for Overhauser dynamic nuclear polarization in solids",

abstract = "Herein, we investigate a novel set of polarizing agents—mixed-valence compounds—by theoretical and experimental methods and demonstrate their performance in high-field dynamic nuclear polarization (DNP) NMR experiments in the solid state. Mixed-valence compounds constitute a group of molecules in which molecular mobility persists even in solids. Consequently, such polarizing agents can be used to perform Overhauser-DNP experiments in the solid state, with favorable conditions for dynamic nuclear polarization formation at ultra-high magnetic fields.",

keywords = "DNP in solids, Overhauser effect, ab initio calculations, mixed valence compounds, molecular dynamics",

author = "Andrei Gurinov and Sieland Benedikt and Andrey Kuzhelev and Hossam Elgabarty and K{\"u}hne, {Thomas D} and Thomas Prisner and Jan Paradies and Marc Baldus and Ivanov, {Konstantin L} and Svetlana Pylaeva",

note = "Funding Information: This work has been supported by iNEXT-Discovery, grant number 871037, funded by the Horizon 2020 program of the European Commission. Svetlana Pylaeva would like to thank Prof. Matvey Fedin, Dr. Yury Lebedev for fruitful discussions of EPR experiments and organic synthesis. HE acknowledges the DFG for funding his temporary position as a principal investigator (Eigene Stelle). TDK acknowledges funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (grant agreement no. 716142). The generous allocation of supercomputer time by the Paderborn Center for Parallel Computing (PC2) is kindly acknowledged. JP acknowledges the DFG for funding (PA1562-14/1). The DNP experiments were supported by the Dutch Research Council (NWO grants 700.11.344 and 700.58.102 to MB). Open access funding enabled and organized by Projekt DEAL. Funding Information: This work has been supported by iNEXT‐Discovery, grant number 871037, funded by the Horizon 2020 program of the European Commission. Svetlana Pylaeva would like to thank Prof. Matvey Fedin, Dr. Yury Lebedev for fruitful discussions of EPR experiments and organic synthesis. HE acknowledges the DFG for funding his temporary position as a principal investigator (Eigene Stelle). TDK acknowledges funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (grant agreement no. 716142). The generous allocation of supercomputer time by the Paderborn Center for Parallel Computing (PC2) is kindly acknowledged. JP acknowledges the DFG for funding (PA1562‐14/1). The DNP experiments were supported by the Dutch Research Council (NWO grants 700.11.344 and 700.58.102 to MB). Open access funding enabled and organized by Projekt DEAL. Publisher Copyright: {\textcopyright} 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH",

year = "2021",

month = jul,

day = "5",

doi = "10.1002/anie.202103215",

language = "English",

volume = "60",

pages = "15371--15375",

journal = "Angewandte Chemie-International Edition",

issn = "1433-7851",

publisher = "John Wiley and Sons Ltd",

number = "28",

}

TY - JOUR

T1 - Mixed-valence compounds as polarizing agents for Overhauser dynamic nuclear polarization in solids

AU - Gurinov, Andrei

AU - Benedikt, Sieland

AU - Kuzhelev, Andrey

AU - Elgabarty, Hossam

AU - Kühne, Thomas D

AU - Prisner, Thomas

AU - Paradies, Jan

AU - Baldus, Marc

AU - Ivanov, Konstantin L

AU - Pylaeva, Svetlana

N1 - Funding Information: This work has been supported by iNEXT-Discovery, grant number 871037, funded by the Horizon 2020 program of the European Commission. Svetlana Pylaeva would like to thank Prof. Matvey Fedin, Dr. Yury Lebedev for fruitful discussions of EPR experiments and organic synthesis. HE acknowledges the DFG for funding his temporary position as a principal investigator (Eigene Stelle). TDK acknowledges funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (grant agreement no. 716142). The generous allocation of supercomputer time by the Paderborn Center for Parallel Computing (PC2) is kindly acknowledged. JP acknowledges the DFG for funding (PA1562-14/1). The DNP experiments were supported by the Dutch Research Council (NWO grants 700.11.344 and 700.58.102 to MB). Open access funding enabled and organized by Projekt DEAL. Funding Information: This work has been supported by iNEXT‐Discovery, grant number 871037, funded by the Horizon 2020 program of the European Commission. Svetlana Pylaeva would like to thank Prof. Matvey Fedin, Dr. Yury Lebedev for fruitful discussions of EPR experiments and organic synthesis. HE acknowledges the DFG for funding his temporary position as a principal investigator (Eigene Stelle). TDK acknowledges funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (grant agreement no. 716142). The generous allocation of supercomputer time by the Paderborn Center for Parallel Computing (PC2) is kindly acknowledged. JP acknowledges the DFG for funding (PA1562‐14/1). The DNP experiments were supported by the Dutch Research Council (NWO grants 700.11.344 and 700.58.102 to MB). Open access funding enabled and organized by Projekt DEAL. Publisher Copyright: © 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH

PY - 2021/7/5

Y1 - 2021/7/5

N2 - Herein, we investigate a novel set of polarizing agents—mixed-valence compounds—by theoretical and experimental methods and demonstrate their performance in high-field dynamic nuclear polarization (DNP) NMR experiments in the solid state. Mixed-valence compounds constitute a group of molecules in which molecular mobility persists even in solids. Consequently, such polarizing agents can be used to perform Overhauser-DNP experiments in the solid state, with favorable conditions for dynamic nuclear polarization formation at ultra-high magnetic fields.

AB - Herein, we investigate a novel set of polarizing agents—mixed-valence compounds—by theoretical and experimental methods and demonstrate their performance in high-field dynamic nuclear polarization (DNP) NMR experiments in the solid state. Mixed-valence compounds constitute a group of molecules in which molecular mobility persists even in solids. Consequently, such polarizing agents can be used to perform Overhauser-DNP experiments in the solid state, with favorable conditions for dynamic nuclear polarization formation at ultra-high magnetic fields.

KW - DNP in solids

KW - Overhauser effect

KW - ab initio calculations

KW - mixed valence compounds

KW - molecular dynamics

UR - http://www.scopus.com/inward/record.url?scp=85107389149&partnerID=8YFLogxK

U2 - 10.1002/anie.202103215

DO - 10.1002/anie.202103215

M3 - Article

C2 - 33908694

SN - 1433-7851

VL - 60

SP - 15371

EP - 15375

JO - Angewandte Chemie-International Edition

JF - Angewandte Chemie-International Edition

IS - 28

ER -

Mixed-valence compounds as polarizing agents for Overhauser dynamic nuclear polarization in solids

Abstract

Bibliographical note

Keywords

Access to Document

Other files and links

Fingerprint

Cite this