In Silico Molecular Engineering of Dysprosocenium-Based Complexes to Decouple Spin Energy Levels from Molecular Vibrations
Molecular nanomagnets hold great promise for spintronics and quantum technologies, provided that their spin memory can be preserved above liquid-nitrogen temperatures. In the past few years, the magnetic hysteresis records observed for two related dysprosocenium-type complexes have highlighted the p...
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| Published in: | The journal of physical chemistry letters Vol. 10; no. 24; p. 7678 |
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| Main Authors: | , , , , , |
| Format: | Journal Article |
| Language: | English |
| Published: |
United States
19.12.2019
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| ISSN: | 1948-7185, 1948-7185 |
| Online Access: | Get more information |
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| Summary: | Molecular nanomagnets hold great promise for spintronics and quantum technologies, provided that their spin memory can be preserved above liquid-nitrogen temperatures. In the past few years, the magnetic hysteresis records observed for two related dysprosocenium-type complexes have highlighted the potential of molecular engineering to decouple vibrational excitations from spin states and thereby enhance magnetic memory. Herein, we study the spin-vibrational coupling in [(Cp
)Dy(Cp*)]
(Cp
= pentaisopropylcyclopentadienyl, Cp* = pentamethylcyclopentadienyl), which currently holds the hysteresis record (80 K), by means of a computationally affordable methodology that combines first-principles electronic structure calculations with a phenomenological ligand field model. Our analysis is in good agreement with the previously reported state-of-the-art ab initio calculations, with the advantage of drastically reducing the computation time. We then apply the proposed methodology to three alternative dysprosocenium-type complexes, extracting physical insights that demonstrate the usefulness of this strategy to efficiently engineer and screen magnetic molecules with the potential of retaining spin information at higher temperatures. |
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| Bibliography: | ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 |
| ISSN: | 1948-7185 1948-7185 |
| DOI: | 10.1021/acs.jpclett.9b02982 |