The Fascinating Journeys of Electrons in the Realm of Nanostructures

In this presentation I would like to invite you follow electrons on their real-time pathways through nanostructured materials. The dynamics of their wave packets relies on excitation state a given nanoparticle and interaction with other electrons even over long distances.

On part of presentation deals with excitation transfer among two semiconductor quantum dots. Here, two complementary theoretical descriptions of the system and dynamics are comparably introduced. On the one hand, small quantum dots are modeled atomistically in the framework of the density-matrix-based time-dependent configuration interaction (ρ-TDCI).¹ Here we were able to observe exciton transfer among the quantum dots including charge separation. On the other hand, an excitation transfer leading to ionization of one quantum dot, the inter-QD Coulomb decay process, was proven with multiconfiguration time-dependent Hartree computations in common QD model potentials for several different classes, numbers, and arrangements of QDs² and give an outlook to a quantum-computer simulation of the same.³      

The other part of the presentation highlights examples of the light-induced electron dynamics of electron-transfer processes among aqueous nanoparticles and the solvent molecules. The workflow is again with ρ-TDCI in atomistic models⁴ with ideas for scale bridging to include solvent molecular dynamics with machine-learning techniques.  

References:

1. Krause, Tremblay, Bande, J. Phys. Chem. A 125 (2021) 4793.
2. Guskov, Langkabel, Berg, Bande, QUARKS: Braz. Electron. J. Phys. Chem. Mat. Sci. 3 (2020) 17.
3. Langkabel, Bande, in preparation.
4. Weber, Tremblay, A. Bande, J. Phys. Chem. C 124 (2020) 26688.