DeNeTheor aims at modeling and simulating light-responsive molecular systems in complex bioenvironments, namely proteins and macromolecular matrices. Excited states and photoinduced dynamics of a series of Re (I) complexes embedded in metallo-labeled mutants of a blue copper protein will be studied.
Depending on the surrounding ligands and on the environment, specific functions, such as electron transfer triggering, luminescent probe or isomerization can be achieved. Novel theoretical tools and multi-scale computational strategies based on quantum mechanics (QM), quantum dynamics (QD), molecular mechanics (MM) and molecular dynamics (MD) will de developed for handling these systems. Spin-vibronic couplings will be considered in the modeling of the dynamics of the isolated chromophores and in the presence of
environments of increasing complexity.
This ambitious goal will be achieved through the combination of three groups with complementary expertise:
(1) the calculation of electronically excited states for transition metal complexes with accurate multireference quantum chemical methods (Strasbourg),

(2) the simulation of dynamical processes with nuclear wavepackets (Strasbourg) and with ab-initio MD (AIMD) methods (Vienna) and

(3) the description of complex biological environments with hybrid QM/MM techniques (Nancy). The expertise of the groups of Strasbourg, Vienna, and Nancy will be combined to develop novel tools and strategies ableĀ  to describe electronic excited states properties and reactivity with enough accuracy. Time evolution of the excited states will be properly described, as well as their interactions with complex surroundings that may tune or modify their properties and dynamics.

The planned consortium will enable collaborative research as well as active exchange of know-how and competences that will lead to the following key achievements:

i) Development of new computational tools suitable to consider biological environments combining QM/MM and AIMD methods, to describe dynamics both in the ground and excited states;

ii) Exploitation of highly accurate QM methods, taking into account spin-orbit and vibronic couplings within the framework of QM/MM approaches;

iii) Production and dissemination of original computational chemistry protocols to model photonic properties and light-induced processes;

iv) Understanding of the interplay between transition metal complexes and biological structures featuring several functions under light control.

Denetheor will greatly enhance the cooperation and transfer of knowledge between the three participating teams and, also very importantly, will promote the participation and qualification of young researcher, involved in each teams. A single team cannot achieve the planned objectives. Instead, this consortium is designed to gather complementary know-how in different competences and will allow for synergetic advances, especially in the field of method development.