Publication date: 17th February 2025
In 2001 I spent a summer at the Chemistry Department of Princeton University (US) thanks to a short-term mobility grant to investigate the electronic and optical properties of a Ruthenium based dye which was been employed in Grätzel or Dye-sensitized solar cells.1 That study was the first of a long series where Density Functional Theory (DFT) and its Time Dependent extension (TDDFT) was used to describe the electronic and optical properties of a metal-based dye and simulate its spectrum in solution. Since that pioneering research to the present, computational modelling based on TDDDFT methods has played a central role in understanding the properties of materials involved in DSSCs and the mechanisms underlying the DSSC functioning. Computational modelling has thus become crucial both in the design of new materials for DSSCs and in their characterization. We focused on metal-organic dyes of Ru(II), Os(II), Cu(I), Fe(II) evaluating the role of solvent in the line-up of molecular orbitals, in the energy of the excited states w.r.t the ground state and in the simulated Uv-vis spectrum.2 The role of spin orbit coupling (SOC) has been explored for Os(II) based dyes and for dyes where Ru(II) experiences a peculiar ligand environment.3 In addition to metallorganic dyes, organic dyes and other constituent materials of DSSCs, such as the electron-hole conductor (Spiro-OMeTAD)4 used in the solid-state version and the dye-sensitized TiO2 nanoparticles5 were investigated. It has been a long and fruitful journey in which interdisciplinary skills have been merged to develop a new technology, and it was from this stimulating environment that perovskite-based solar cells were born.
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