Excited-states of a rhenium carbonyl diimine complex: solvation models, spin-orbit coupling, and vibrational sampling effects

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Excited-states of a rhenium carbonyl diimine complex: solvation models, spin-orbit coupling, and vibrational sampling effects

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Title: Excited-states of a rhenium carbonyl diimine complex: solvation models, spin-orbit coupling, and vibrational sampling effects
Author: Mai, Sebastian; Gattuso, Hugo; Fumanal, María; Muñoz Losa, Aurora; Monari, Antonio; Daniel, Chantal; Gonzalez Herrero, Leticia
Abstract: Presentamos una investigación química cuántica de los estados excitados del complejo [Re (CO) 3 (Im) (Phen)] + (Im = imidazol; Phen = 1,10-fenantrolina) en solución que incluye acoplamientos de giro-órbita y muestreo vibracional. Para este objetivo, implementamos la mecánica cuántica / mecánica molecular (QM / MM) de incrustación electrostática en el conjunto de programas funcionales de densidad de Ámsterdam, adecuados para cálculos funcionales de densidad dependientes del tiempo que incluyen acoplamientos de órbita de espín. La nueva implementación se emplea para simular el espectro de absorción del complejo, que se compara con los resultados de la solvatación continua implícita y la inclusión de densidad congelada. Se utilizan simulaciones de dinámica molecular para muestrear las conformaciones del estado fundamental en la solución. Los resultados demuestran que cualquier estudio de los estados excitados de [Re (CO) 3 (Im) (Phen)] + en solución y su dinámica debe incluir un muestreo extenso de movimiento vibracional y acoplamientos de giro-órbita.We present a quantum-chemical investigation of the excited states of the complex [Re(CO)3(Im)(Phen)]+ (Im = imidazole; Phen = 1,10-phenanthroline) in solution including spin–orbit couplings and vibrational sampling. To this aim, we implemented electrostatic embedding quantum mechanics/molecular mechanics (QM/MM) in the Amsterdam Density Functional program suite, suitable for time-dependent density functional calculations including spin–orbit couplings. The new implementation is employed to simulate the absorption spectrum of the complex, which is compared to the results of implicit continuum solvation and frozen-density embedding. Molecular dynamics simulations are used to sample the ground state conformations in solution. The results demonstrate that any study of the excited states of [Re(CO)3(Im)(Phen)]+ in solution and their dynamics should include extensive sampling of vibrational motion and spin–orbit couplings.
URI: http://hdl.handle.net/10662/8982
Date: 2017


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