Toward Fast and Accurate Evaluation of Charge On-Site Energies and Transfer Integrals in Supramolecular Architectures Using Linear Constrained Density Functional Theory (CDFT)-Based Methods

Laura E. Ratcliff (1) , Luca Grisanti (2) , Luigi Genovese (1) , Thierry Deutsch (1) , Tobias Neumann (3) , Denis Danilov (3) , Wolfgang Wenzel (3) , David Beljonne (2) , Jérôme Cornil (2)

1 LSIM - Laboratory of Atomistic Simulation
2 Laboratory for Chemistry of Novel Materials
3 Karlsruhe Nano Micro Facility

A fast and accurate scheme has been developed to evaluate two key molecular parameters (on-site energies and transfer integrals) that govern charge transport in organic supramolecular architecture devices. The scheme is based on a constrained density functional theory (CDFT) approach implemented in the linear-scaling BigDFT code that exploits a wavelet basis set. The method has been applied to model disordered structures generated by force-field simulations. The role of the environment on the transport parameters has been taken into account by building large clusters around the active molecules involved in the charge transfer.

Mots clés: Light-Emitting Devices; Organic Semiconductors; Global Optimization; Electron-Transfer; Transport; Clusters; Glasses

Domaines: Physique [physics]

Laura E. Ratcliff, Luca Grisanti, Luigi Genovese, Thierry Deutsch, Tobias Neumann, et al.. Toward Fast and Accurate Evaluation of Charge On-Site Energies and Transfer Integrals in Supramolecular Architectures Using Linear Constrained Density Functional Theory (CDFT)-Based Methods. Journal of Chemical Theory and Computation, 2015, 11 (5), pp.2077-2086. ⟨10.1021/acs.jctc.5b00057⟩. ⟨hal-01616553⟩