Ultrafast intersystem crossings in Fe-Co Prussian blue analogues
Abstract Ultrafast spincrossover is studied in Fe-Co Prussian blue analogues using a dissipative quantum-mechanical model of a cobalt ion coupled to a breathing mode. All electronic interactions are treated on an equal footing. It is theoretically demonstrated that the divalent cobalt ion reaches 90...
Guardado en:
| Autor principal: | |
|---|---|
| Formato: | article |
| Lenguaje: | EN |
| Publicado: |
Nature Portfolio
2017
|
| Materias: | |
| Acceso en línea: | https://doaj.org/article/50dad9edc11f42598e4fd9de03baa9eb |
| Etiquetas: |
Agregar Etiqueta
Sin Etiquetas, Sea el primero en etiquetar este registro!
|
| Sumario: | Abstract Ultrafast spincrossover is studied in Fe-Co Prussian blue analogues using a dissipative quantum-mechanical model of a cobalt ion coupled to a breathing mode. All electronic interactions are treated on an equal footing. It is theoretically demonstrated that the divalent cobalt ion reaches 90% of the $$S{\boldsymbol{=}}\frac{{\bf{3}}}{{\bf{2}}}$$ S = 3 2 value within 20 fs after photoexciting a low-spin Co3+ ion by an iron-to-cobalt charge transfer. The doublet-to-quartet spin crossover is significantly faster than the oscillation period of the breathing mode. The system relaxes to the lowest manifold of divalent cobalt (4 T 1) in 150–200 fs. Strong oscillations in spin-orbit coupling and the involvement of higher-lying quartets are found. |
|---|