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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Vydáno v:The journal of physical chemistry letters Ročník 10; číslo 24; s. 7678
Hlavní autoři: Ullah, Aman, Cerdá, Jesús, Baldoví, José J, Varganov, Sergey A, Aragó, Juan, Gaita-Ariño, Alejandro
Médium: Journal Article
Jazyk:angličtina
Vydáno: United States 19.12.2019
ISSN:1948-7185, 1948-7185
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Shrnutí: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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ISSN:1948-7185
1948-7185
DOI:10.1021/acs.jpclett.9b02982