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Title: Exploring the Vibrational Side of Spin-Phonon Coupling in Single-Molecule Magnets via 161Dy Nuclear Resonance Vibrational Spectroscopy

Abstract

Synchrotron-based nuclear resonance vibrational spectroscopy (NRVS) using the Mossbauer isotope 161Dy has been employed for the first time to study the vibrational properties of a single-molecule magnet (SMM) incorporating DyIII, namely [Dy(Cy3PO)(2)(H2O)(5)]Br-3•2 (Cy3PO)•2 H2O•2 EtOH. The experimental partial phonon density of states (pDOS), which includes all vibrational modes involving a displacement of the DyIII ion, was reproduced by means of simulations using density functional theory (DFT), enabling the assignment of all intramolecular vibrational modes. This study proves that 161Dy NRVS is a powerful experimental tool with significant potential to help to clarify the role of phonons in SMMs.

Authors:
ORCiD logo [1];  [2];  [1];  [1];  [1];  [3];  [4];  [4];  [4]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [5]; ORCiD logo [1]
  1. Department of PhysicsTechnische Universität Kaiserslautern Erwin-Schrödinger-Str. 46 67663 Kaiserslautern Germany
  2. Institute of Inorganic ChemistryKarlsruhe Institute of Technology Engesserstr. 15 76131 Karlsruhe Germany
  3. Advanced Photon SourceArgonne National Laboratory 9700 South Cass Avenue Argonne IL 60439 USA, Department of PhysicsUniversity of Alabama at Birmingham Birmingham AL 35294 USA
  4. Advanced Photon SourceArgonne National Laboratory 9700 South Cass Avenue Argonne IL 60439 USA
  5. Institute of Inorganic ChemistryKarlsruhe Institute of Technology Engesserstr. 15 76131 Karlsruhe Germany, Institute of NanotechnologyKarlsruhe Institute of Technology 76021 Karlsruhe Germany
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); German Research Foundation (DFG); Consortium for Materials Properties Research in Earth Sciences (COMPRES); National Science Foundation (NSF)
OSTI Identifier:
1616193
Alternate Identifier(s):
OSTI ID: 1616195; OSTI ID: 1631809
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Published Article
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition) Journal Volume: 59 Journal Issue: 23; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
Germany
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; dysprosium; nuclear resonance vibrational spectroscopy; phonons; single-molecule magnets

Citation Formats

Scherthan, Lena, Pfleger, Rouven F., Auerbach, Hendrik, Hochdörffer, Tim, Wolny, Juliusz A., Bi, Wenli, Zhao, Jiyong, Hu, Michael Y., Alp, E. Ercan, Anson, Christopher E., Diller, Rolf, Powell, Annie K., and Schünemann, Volker. Exploring the Vibrational Side of Spin-Phonon Coupling in Single-Molecule Magnets via 161Dy Nuclear Resonance Vibrational Spectroscopy. Germany: N. p., 2020. Web. https://doi.org/10.1002/anie.201914728.
Scherthan, Lena, Pfleger, Rouven F., Auerbach, Hendrik, Hochdörffer, Tim, Wolny, Juliusz A., Bi, Wenli, Zhao, Jiyong, Hu, Michael Y., Alp, E. Ercan, Anson, Christopher E., Diller, Rolf, Powell, Annie K., & Schünemann, Volker. Exploring the Vibrational Side of Spin-Phonon Coupling in Single-Molecule Magnets via 161Dy Nuclear Resonance Vibrational Spectroscopy. Germany. https://doi.org/10.1002/anie.201914728
Scherthan, Lena, Pfleger, Rouven F., Auerbach, Hendrik, Hochdörffer, Tim, Wolny, Juliusz A., Bi, Wenli, Zhao, Jiyong, Hu, Michael Y., Alp, E. Ercan, Anson, Christopher E., Diller, Rolf, Powell, Annie K., and Schünemann, Volker. Tue . "Exploring the Vibrational Side of Spin-Phonon Coupling in Single-Molecule Magnets via 161Dy Nuclear Resonance Vibrational Spectroscopy". Germany. https://doi.org/10.1002/anie.201914728.
@article{osti_1616193,
title = {Exploring the Vibrational Side of Spin-Phonon Coupling in Single-Molecule Magnets via 161Dy Nuclear Resonance Vibrational Spectroscopy},
author = {Scherthan, Lena and Pfleger, Rouven F. and Auerbach, Hendrik and Hochdörffer, Tim and Wolny, Juliusz A. and Bi, Wenli and Zhao, Jiyong and Hu, Michael Y. and Alp, E. Ercan and Anson, Christopher E. and Diller, Rolf and Powell, Annie K. and Schünemann, Volker},
abstractNote = {Synchrotron-based nuclear resonance vibrational spectroscopy (NRVS) using the Mossbauer isotope 161Dy has been employed for the first time to study the vibrational properties of a single-molecule magnet (SMM) incorporating DyIII, namely [Dy(Cy3PO)(2)(H2O)(5)]Br-3•2 (Cy3PO)•2 H2O•2 EtOH. The experimental partial phonon density of states (pDOS), which includes all vibrational modes involving a displacement of the DyIII ion, was reproduced by means of simulations using density functional theory (DFT), enabling the assignment of all intramolecular vibrational modes. This study proves that 161Dy NRVS is a powerful experimental tool with significant potential to help to clarify the role of phonons in SMMs.},
doi = {10.1002/anie.201914728},
journal = {Angewandte Chemie (International Edition)},
number = 23,
volume = 59,
place = {Germany},
year = {2020},
month = {3}
}

Journal Article:
Free Publicly Available Full Text
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https://doi.org/10.1002/anie.201914728

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