Simulation of electronic excitation and emission spectra using advanced molecular dynamics combined with TDDFT.

01 January 2014 → 31 December 2019
Research Foundation - Flanders (FWO)
Research disciplines
  • Natural sciences
    • Classical physics
    • Elementary particle and high energy physics
    • Other physical sciences
electronic excitation and emission spectra TD-DFT molecular dynamics
Project description

Spectroscopy involving electronic excited states aims at providing insight into the electronic structure and light-matter interactions of materials. New theoretical developments, such as time-dependent density functional theory (TD-DFT), enable the study of large systems containing up to 400 atoms. Here, we will combine detailed electronic structure methods – and in particular the popular TD-DFT method – with the exploration of energy surfaces using advanced molecular dynamics (MD). This approach is innovative and opens possibilities to an in-depth analysis of computed optical spectra since MD accounts for temperature and solvent effects, as well as for the flexibility of the substrates under study. The systems of interest are large dyes and metal-functionalized organic linkers present in porous materials such as Metalorganic frameworks (MOFs).
We will compute adiabatic absorption spectra of compounds in different complex molecular environments; in particular in vacuo, in a solvent and in aggregated form. Luminescence spectra, which involve the challenging optimization of the excited state, will also be investigated. Sophisticated multi-layer simulations will be performed thereby assessing a static versus a dynamic approach. Throughout the project, there will be a close collaboration with experimental partners. Our goal is to link spectral changes with geometrical parameters and as such contribute to the rational design of compounds exhibiting specific electronic features.