Our research focusses on the development and the applications of theoretical methods for simulating the dynamics of molecules beyond the Born-Oppenheimer approximation, i.e., when the coupling between electronic and nuclear motion cannot be neglected and leads to the appearance of the so-called nonadiabatic effects. The breakdown of the Born-Oppenheimer approximation is common for photoinduced and electron-transfer processes, e.g. photochemical reactions, photosynthesis, solar cells, retinal isomerization in the primary step of vision, chemiluminescence, or in atmospheric chemistry, and leads to fascinating phenomena. In fact, nonadiabatic effects are ubiquitous as soon as a given chemical process requires more than one electronic state for its description, but their theoretical description remains an important and arduous challenge due to the necessity of revisiting several critical approximations commonly employed in theoretical chemistry.
The main pillars of our scientific research are the development and the application of theoretical methods for studying the dynamics of molecules in their electronically excited states.
We are currently working on the development of a hierarchy of nonadiabatic methods centered around trajectory-guided techniques, such as full multiple spawning, with a controllable degree of accuracy. We are not only interested in the accuracy of the nuclear dynamics per se, but also in the inclusion of different additional factors contributing to a precise description of the excited-state dynamics, such as external fields, environment, or relativistic effects.
We also employ the formalism of the Exact Factorization to study the ultrafast funneling processes of photoexcited molecular systems.
Applications of nonadiabatic dynamics
We apply nonadiabatic techniques to the study of transient molecules of first importance for atmospheric chemistry and to study excited-state processes in energy-related devices. We also intensively collaborate with experimental groups to employ a broad panel of theoretical techniques to study real chemical problems and to provide a theoretical support for the analysis of complex experimental data.
National and international collaborators
- Dr. Federica Agostini (France) – Exact Factorization
- Dr. Benoît Mignolet (Belgium) – Ab Initio Multiple Spawning
- Dr. Tom J. Penfold (UK) – Nonadiabatic dynamics
- Prof. Petr Slavíček (Czech Republic) – Nonadiabatic dynamics
- Prof. Todd J. Martínez (US) – Full and Ab Initio Multiple Spawning
- Dr. Tom A. A. Oliver (UK) – Ultrafast dynamics
- Prof. Andrew J. Orr-Ewing (UK) – Ultrafast dynamics and Atmospheric chemistry
- Prof. Mike N. R. Ashfold (UK) – Ultrafast dynamics
Poster for the Postgraduate open days at Durham University.