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

Scherthan, Lena; Pfleger, Rouven F. ORCID iD icon 1; Auerbach, Hendrik; Hochdörffer, Tim; Wolny, Juliusz A.; Bi, Wenli; Zhao, Jiyong; Hu, Michael Y.; Alp, E. Ercan; Anson, Christopher E. 1; Diller, Rolf; Powell, Annie K. 1,2; Schünemann, Volker
1 Institut für Anorganische Chemie (AOC), Karlsruher Institut für Technologie (KIT)
2 Institut für Nanotechnologie (INT), Karlsruher Institut für Technologie (KIT)

Abstract:

Bad vibrations? $^{161}$Dy nuclear resonance vibrational spectroscopy gives direct experimental access to the partial phonon density of states which includes all vibrational modes involving a displacement of the Dy$^{III}$ ion. In combination with density functional theory, an assignment to all intramolecular vibrational modes is possible, paving an ideal path to help to clarify the role of phonons in single-molecule magnets.

Synchrotron-based nuclear resonance vibrational spectroscopy (NRVS) using the Mössbauer isotope $^{161}$Dy has been employed for the first time to study the vibrational properties of a single-molecule magnet (SMM) incorporating Dy$^{III}$, namely [Dy(Cy$_{3}$PO)$_{2}$(H$_{2}$O)$_{5}$]Br$_{3}$⋅2 (Cy$_{3}$PO)⋅2 H$_{2}$O ⋅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 $^{161}$Dy NRVS is a powerful experimental tool with significant potential to help to clarify the role of phonons in SMMs.


Verlagsausgabe §
DOI: 10.5445/IR/1000119853
Veröffentlicht am 28.11.2021
Originalveröffentlichung
DOI: 10.1002/anie.201914728
Scopus
Zitationen: 7
Web of Science
Zitationen: 6
Dimensions
Zitationen: 8
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Anorganische Chemie (AOC)
Institut für Nanotechnologie (INT)
Publikationstyp Zeitschriftenaufsatz
Publikationsmonat/-jahr 06.2020
Sprache Englisch
Identifikator ISSN: 1433-7851, 1521-3773
KITopen-ID: 1000119853
HGF-Programm 43.21.04 (POF III, LK 01) Molecular Engineering
Erschienen in Angewandte Chemie / International edition
Verlag John Wiley and Sons
Band 59
Heft 23
Seiten 8818–8822
Vorab online veröffentlicht am 17.03.2020
Nachgewiesen in Dimensions
Web of Science
Scopus
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