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Chromone-methanol clusters in the electronic ground and lowest triplet state: a delicate interplay of non-covalent interactions.
Boden, Pol; Strebert, Patrick H; Meta, Marcel; Dietrich, Fabian; Riehn, Christoph; Gerhards, Markus.
Afiliación
  • Boden P; Fachbereich Chemie & State Research Center OPTIMAS, TU Kaiserslautern, Erwin-Schrödinger-Str. 52, D-67663 Kaiserslautern, Germany.
  • Strebert PH; Fachbereich Chemie & State Research Center OPTIMAS, TU Kaiserslautern, Erwin-Schrödinger-Str. 52, D-67663 Kaiserslautern, Germany.
  • Meta M; Fachbereich Chemie & State Research Center OPTIMAS, TU Kaiserslautern, Erwin-Schrödinger-Str. 52, D-67663 Kaiserslautern, Germany.
  • Dietrich F; Fachbereich Chemie & State Research Center OPTIMAS, TU Kaiserslautern, Erwin-Schrödinger-Str. 52, D-67663 Kaiserslautern, Germany.
  • Riehn C; Núcleo Milenio MultiMat & Departamento de Ciencias Físicas, Universidad de La Frontera, Temuco, Chile. fabian.dietrich@ufrontera.cl.
  • Gerhards M; Fachbereich Chemie & State Research Center OPTIMAS, TU Kaiserslautern, Erwin-Schrödinger-Str. 52, D-67663 Kaiserslautern, Germany.
Phys Chem Chem Phys ; 24(25): 15208-15216, 2022 Jun 29.
Article en En | MEDLINE | ID: mdl-35579075
Chromone offers two energetically almost equivalent docking sites for alcohol molecules, in which the hydroxyl group is hydrogen bonded to one of the free electron pairs of the carbonyl O atom. Here, the delicate balance between these two competing arrangements is studied by combining IR/R2PI and UV/IR/UV spectroscopy in a molecular beam supported by quantum-chemical calculations. Most interestingly, chromone undergoes an efficient intersystem crossing into the triplet manifold upon electronic excitation, so that the studies on aromatic molecule-solvent complexes are for the first time extended to such a cluster in a triplet state. As the lowest triplet state (T1) is of ground state character, powerful energy decomposition approaches such as symmetry-adapted perturbation theory (SAPT) and local energy decomposition using the domain-based local pair natural orbital coupled-cluster method (DLPNO-CCSD(T)/LED) are applied. From the theoretical analysis we infer for the T1 state a loss of planarity (puckering) of the 4-pyrone ring of the chromone unit, which considerably affects the interplay between different types of non-covalent interactions at the two possible binding sites.
Asunto(s)

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Cromonas / Metanol Idioma: En Revista: Phys Chem Chem Phys Asunto de la revista: BIOFISICA / QUIMICA Año: 2022 Tipo del documento: Article País de afiliación: Alemania Pais de publicación: Reino Unido

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Cromonas / Metanol Idioma: En Revista: Phys Chem Chem Phys Asunto de la revista: BIOFISICA / QUIMICA Año: 2022 Tipo del documento: Article País de afiliación: Alemania Pais de publicación: Reino Unido