Theoretical description of electronic excitations in extended systems: beyond the static material model
The theoretical description of bistable materials requires dealing with the interplay of various phenomena, like temperature, environmental effects and electron correlation. We developed a procedure to combine the benefits of the molecular dynamics techniques with the accuracy of the ab initio wave...
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| Tipo de recurso: | tesis doctoral |
| Estado: | Versión publicada |
| Fecha de publicación: | 2011 |
| País: | España |
| Institución: | CBUC, CESCA |
| Repositorio: | TDR. Tesis Doctorales en Red |
| OAI Identifier: | oai:www.tdx.cat:10803/51760 |
| Acceso en línea: | http://hdl.handle.net/10803/51760 |
| Access Level: | acceso abierto |
| Palabra clave: | Química Teórica Química computacional Espectroscopía Dinámica Molecular theoretical Chemistry Computational chemistry Spectroscopy Molecular dynamics 54 544 |
| Sumario: | The theoretical description of bistable materials requires dealing with the interplay of various phenomena, like temperature, environmental effects and electron correlation. We developed a procedure to combine the benefits of the molecular dynamics techniques with the accuracy of the ab initio wave function based methods including various models for the surroundings. The combination of these computational methods involved the making of specific software tools. The proposed procedure has been applied successfully, obtaining good agreements with experimental data, on organic molecules in solvent (cytosine tautomers in water), crystalline materials (NiO, LaMnO3 and TTTA) and inorganic spin-crossover compounds (FeII(bpy)3). We achieved a significant improvement in the description of their absorption spectra: including ligand-to-metal and metal-to-metal charge transfer processes, formally dipole forbidden transitions and the broadening of the spectral bands. Moreover, we observe dramatic changes on the electronic structure by incorporating the environmental effects on the theoretical model. |
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