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Accueil > EN > Recruitment > PhD project

Fully atomistic simulation of the interaction of environmentally relevant molecules with soot particles.

par Johanna Leclercq - publié le

Title of the PhD project :
Fully atomistic simulation of the interaction of environmentally relevant molecules with soot particles.

Name of the PhD Director : Daniel PELAEZ RUIZ
Name of the co-director or collaborator : Denis DUFLOT

Laboratory : PhLAM

Financial supports : U. Lille

Identified Research Programmes : CaPPA, CLIMIBIO

Summary of the PhD project :
The goal of this Ph.D. is the characterisation, at a molecular level, of the adsorption and desorption processes of atmospherically relevant molecules (OH, NO2, small Polycyclic Aromatic Hydrocarbons,…) adsorbed on atmopsherical particles (soot, black carbon,…) as well as the simulation of the spectroscopical signatures leading to their experimental determination.

The novelty of this project lies in the use of mixed quantum-classical scheme enabling the simulation of very different spatial and temporal scales. We shall describe at a fully quantum level (electrons and nuclei) both molecule and local environment. To this end, we shall make use of molecular quantum dynamical methods related to the Multiconfiguration Time-Dependent Hartree (MCTDH) algorithm [1]. This method, which is numerically exact, allows the computation of molecular spectra in very good agreement with experience [2]. This accuracy, however, depends on the quality of the description of the molecular interactions (electronic structure). The computational cost of this grows exponentially with system size. To circumvent this issue, we shall complete the modelling of the extended system (aerosol) by using a hierarchical quantum-classical approach (QM/MM) specific for aerosol particles which has been recently validated in our group [3] together with our recent fully automated technique for the characterisation of internolecular interactions [4]. A collaboration with the experimental group of C. Focsa and C. Pirim (PMI, PhLAM) will be also set up during the thesis.

References :
[1] M. H. Beck, A. Jäckle, G. A. Worth, H.-D. Meyer, Phys. Rep. 324, 1 (2000).
[2] D. Peláez, H.-D. Meyer, Chem. Phys. 482, 100 (2017).
[3] C. R. Fotsing Kwetche, C. Toubin, D. Duflot, (submitted) (2019).
[4] S. Kopec, E. Martínez-Núñez, J. Soto, D. Peláez, (in revision) (2019).