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2024-11-21

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cc-by-nc (c) Santiago, Raul et al., 2024
Si us plau utilitzeu sempre aquest identificador per citar o enllaçar aquest document: https://hdl.handle.net/2445/229529

Rational design of organic diradicals with robust high-spin ground state based on antiaromatic linkers

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https://doi.org/10.1039/d4sc05225k

Resum

Fully-organic molecules with high-spin ground states are promising building blocks for new lightweight flexible magnetic materials for emerging technological applications (e.g. spintronics). In this study, we explore the potential of diradicals made of two diphenylmethyl-based open-shell cores covalently linked via different types of pentalene and diazapentalene-based antiaromatic couplers (including dibenzopentalenes and acene-inserted derivatives). Accurate electronic structure calculations have been employed to target non-bonding and non-disjoint frontier molecular orbitals that favor high-spin configurations, leading to the identification of diradicals displaying robust triplet ground states. These candidates exhibit singlet-triplet energy gaps that are up to ten times the thermal energy at room temperature. These substantial gaps emerge from strong interactions between the p-systems of the open-shell centers and the antiaromatic coupler. These interactions not only result in high spin states but are also found to lead to an enhanced stability of the diradicals by drastically dampening their inherent antiaromatic character as compared to the bare couplers, and promoting a high degree of spin density delocalization. These findings highlight the potential of pentalene-based diradicals as building blocks for developing new advanced fully organic magnetic materials.

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Estructura electrònica, Enllaços químics, Química orgànica, Materials magnètics

Matèries (anglès)

Electronic structure, Chemical bonds, Organic chemistry, Magnetic materials

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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))
Articles publicats en revistes (Química Inorgànica i Orgànica)

Citació

SANTIAGO, Raul, et al. Rational design of organic diradicals with robust high-spin ground state based on antiaromatic linkers. Chemical Science. 2024. Vol. 16, num. 1, pags. 430-447. ISSN 2041-6520. [consulted: 25 of May of 2026]. Available at: https://hdl.handle.net/2445/229529

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