Exchange controlled triplet fusion in metal-organic frameworks.
Nat Mater
; 21(11): 1275-1281, 2022 11.
Article
em En
| MEDLINE
| ID: mdl-36202994
ABSTRACT
Triplet-fusion-based photon upconversion holds promise for a wide range of applications, from photovoltaics to bioimaging. The efficiency of triplet fusion, however, is fundamentally limited in conventional molecular and polymeric systems by its spin dependence. Here, we show that the inherent tailorability of metal-organic frameworks (MOFs), combined with their highly porous but ordered structure, minimizes intertriplet exchange coupling and engineers effective spin mixing between singlet and quintet triplet-triplet pair states. We demonstrate singlet-quintet coupling in a pyrene-based MOF, NU-1000. An anomalous magnetic field effect is observed from NU-1000 corresponding to an induced resonance between singlet and quintet states that yields an increased fusion rate at room temperature under a relatively low applied magnetic field of 0.14 T. Our results suggest that MOFs offer particular promise for engineering the spin dynamics of multiexcitonic processes and improving their upconversion performance.
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1
Coleções:
01-internacional
Base de dados:
MEDLINE
Assunto principal:
Estruturas Metalorgânicas
Idioma:
En
Ano de publicação:
2022
Tipo de documento:
Article