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2023

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cc-by-nd (c) Vela, S. et al., 2023
Si us plau utilitzeu sempre aquest identificador per citar o enllaçar aquest document: https://hdl.handle.net/2445/225250

Understanding Kinetically Controlled Spin Transitions in Bistable Spin Crossover Materials

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Recurs relacionat

https://doi.org/10.1039/D2TC04266E

Resum

Spin crossover (SCO) materials can be kinetically trapped in a photo-excited metastable state in the so-called LIESST and reverse-LIESST processes. Under these conditions, SCO molecules are excellent light-responsive bistable molecular switches. However, above a certain temperature (TLIESST and Tr-LIESST, respectively), the relaxation to the ground state becomes favorable and their bistability is suppressed. Understanding the mechanism of these processes, and being able to predict their kinetics, is key to designing SCO switches that are able to operate at room temperature. Herein, we reveal the mechanism of thermally induced spin transitions of the [FeII(1-bpp)2]2+ SCO complex, and we predict its TLIESST (as well as its T1/2) with unprecedented accuracy. This is possible here thanks to the efficient reconstruction of the low-spin (LS, S = 0), high-spin (HS, S = 2) and intermediate (IS, S = 1) state Free energy surfaces (FESs) with ab initio and machine-learning methods, and the characterization of the minimum energy crossing points (MECPs) connecting those FESs. This approach paves the way for the systematic investigation of molecular features determining the mechanism of kinetically controlled transitions in SCO materials, as well as their temperature-dependent rate constants.

Matèries

Cinètica química, Ciència dels materials, Compostos de coordinació

Matèries (anglès)

Chemical kinetics, Materials science, Coordination compounds

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Articles publicats en revistes (Ciència dels Materials i Química Física)
Articles publicats en revistes (Institut de Química Teòrica i Computacional (IQTCUB))

Citació

VELA LLAUSÍ, Sergi, FUMANAL QUINTANA, María, SOUSA ROMERO, Carmen. Understanding Kinetically Controlled Spin Transitions in Bistable Spin Crossover Materials. _Journal of Materials Chemistry C_. 2023. Vol. 11, núm. 235-243. [consulta: 26 de gener de 2026]. ISSN: 2050-7526. [Disponible a: https://hdl.handle.net/2445/225250]

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