L-to-R: Pablo, Alessandro, Michele, Ruslan
Our research is divided into two main topics: dynamics of charge and excitation energy transfer, and subsystem DFT method development. We pursue state-of-the-art theory development as well as cutting-edge applications related to photosynthesis, design of novel materials for molecular electronics, electron transfer in biosystems and molecule-surface interactions.
Non-Adiabatic Dynamics with Subsystem DFT
This project involves development of electronic structure methods to carry out non-adiabatic molecular dynamics simulations in the framework of subsystem DFT. The code development for this project will take place within ADF and Quantum ESPRESSO suites of softwares.
The new methods will be applied to a range of problems:
- Electron and exciton transfer in biosystems
- Dye sensitized solar cells
- Organic-Metal and Organic-Semiconductor interfaces
Non-Local Potentials for Subsystem DFT
Interactions between subsystems, covalent bonds as well as weak van der
Waals, are tough to get with Susbsystem DFT.
This project involves development of non-local orbital-free and
orbital-dependent embedding potentials for the
correct treatment of these interactions between subsystems.
Van der Waals Interactions in Subsystem DFT
Subsystem DFT offers the perfect theoretical framework for the definition of van der Waal interactions between molecules. This project involves development of
- Self-consistent embedding potentials for the correct treatment of long-range interactions between subsystems.
- Post-SCF energy corrections based on fluctuation-dissipation theorem in DFT and the Casimir-Polder/Longuet-Higgins formula of vdW interactions.
High-Accuracy Theoretical Spectroscopy of Small Molecules
In this project we push ab-initio electronic structure to its limits.
Using Explicitly Correlated Gaussians (ECG) we will describe the electronic structure of
small molecules very accurately. This will allow us to calculate spectra of molecules
for which experiments are lagging behind. The calculated spectra will have an enormous
impact in astrochemistry and astrophysics as well as in spectroscopy.
This project will span a number of techniques, from many-body perturbation theory, response theory, and post-Born-Oppenheimer corrections.
Charge transfer couplings and excitations with subsytem DFT
Implementation in ADF of electronic couplings in the context of Subsystem Density-Functional Theory (specifically the FDE formulation). Results published in JCP.
Hole conduction in wet and dry DNA
The real-time monitoring of the movement of a hole along DNA is carried out with molecular dynamics of the fully solvated DNA+ radical cation. The dinamics include an evaluation of the likelihoodof the hole to transfer from one nucleobase to an adjacent one. The code involve force field switching of neutral/cationic nucleobases as the hole is transferred. Results published in JPCB.
A comprehensive PES of H3+
42,500 ab-initio energies of the molecular ion H3+ were calculated with a in-house FORTRAN code to a sub 0.01-wavenumber precision. Results were published in several JCP articles and one PRL letter.
Calculation of the electric field gradient (EFG) at the nuclei
EFGs were calculated in H2. After vibrational averaging, the calculations were extended on D2 and HD. We derived the most accurate to date quadrupole constant of the deuteron. Results published in PRA.
Charge transfer in endohedral complexes of Lithium and Fullerene C60
The ability of C60 to accept electrons from encapsulated Lithium atoms was analyzed. It was found that the Coulomb interaction between charged Li and the fullerene cage is responsible for the stability of complexes having 3 or more excess electrons on C60. The results are published in CPL.