Artículo
The deposition of the spin crossover Fe(II)-pyrazolylborate complex on Au(111) surface at molecular level
Autor/es | Montenegro-Pohlhammer, Nicolás
Sánchez de Armas, María Rocío Jiménez Calzado, Carmen |
Departamento | Universidad de Sevilla. Departamento de Química Física |
Fecha de publicación | 2021 |
Fecha de depósito | 2024-01-18 |
Publicado en |
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Resumen | The interaction at molecular level of the spin-crossover FeII((3,5-(CH3)2Pz)3BH)2 complex with
the Au(111) surface is analyzed by means of rPBE periodic calculations. Our results show that
the adsorption on the metallic ... The interaction at molecular level of the spin-crossover FeII((3,5-(CH3)2Pz)3BH)2 complex with the Au(111) surface is analyzed by means of rPBE periodic calculations. Our results show that the adsorption on the metallic surface enhances the transition energy, increasing the relative stability of the low spin (LS) state. The interaction indeed is spin-dependent, stronger for the low spin than the high spin (HS) state. The different strength of the Fe ligand field at low and high temperature manifests on the nature, spatial extension and relative energy of the states close to the Fermi level, with a larger metal-ligand hybridization in the LS state. This feature is of relevance for the differential adsorption of the LS and HS molecules, the spin-dependent conductance, and for the differences found in the corresponding STM images, correctly reproduced from the density of states provided by the rPBE calculations. It is expected that this spin dependence will be a general feature of the SCO molecule-substrate interaction, since it is rooted in the different ligand field of Fe site at low and high temperatures, a common hallmark of the Fe(II) SCO complexes. Finally, the states involved in the LIESST phenomenon has been identify through NEVPT2 calculations on a model reaction path. A tentative pathway for the photoinduced LS--> HS transition is proposed, that does not involve the intermediate triplet states, and nicely reproduces both the blue laser wavelength required for the activation, and the wavelength of the reverse HS -> LS transition. |
Agencias financiadoras | Agencia Estatal de Investigación. España Ministerio de Ciencia e Innovación (MICIN). España European Commission (EC). Fondo Europeo de Desarrollo Regional (FEDER) |
Identificador del proyecto | PGC2018-101689-B-I00 |
Cita | Montenegro-Pohlhammer, N., Sánchez de Armas, M.R. y Jiménez Calzado, C. (2021). The deposition of the spin crossover Fe(II)-pyrazolylborate complex on Au(111) surface at molecular level. Chemistry A European Journal, 27 (2), 712-727. https://doi.org/10.1002/chem.202003520. |
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