The project activity has been organized in different research lines, that are here summarized together with the main results obtained for each line.
1. Development of a computational approach and the related software to simulate in real time the behavior of plasmons simulated within classical electromagnetic theory. During this period the basic approach to perform this task has been elaborated and implemented in a specific software code called TDPlas. The latter is currently private, will be made public by the end of the project.
Main results achieved along this line: open source, public version of the code TDPlas, that is able to simulate, within the approximations intrinsic in the model, the time evolutions of plasmons supported by metal nanoparticle, taking into account the chemical nature of the metal, the shape of the metal nanoparticle and the dielectric nature of the environment.
2. Interfacing the modeling of plasmons with that of molecules, based on an atomistic quantum mechanics descriptions. The interface has been created for one of the most common quantum mechanical approaches to describe electronic states of molecule, and has been expanded to treat exquisitely quantum mechanical effects such as decoherence and relaxation. The theory has been implemented in a scientific software (WaveT) that has been also made suitable to run on the supercomputers available in EU national supercomputer centers, thanks to a specific EU high-performance computer grant called PRACE preparatory access. Main results achieved along this line: open source, public version of the scientific code WaveT and its interface with TDPlas, parallelized to make possible the use of high performance supercomputers.
3. Development of theory and implementation to study light-triggered chemical reactions when both the molecule and the plasmons behave quantum mechanically. This has been performed so far with a model description of plasmons and a dynamical, atomistic description of molecule. Main results achieved along this line: extension of an existing quantum chemistry code to treat molecule coupled to quantum plasmons; first ever simulation of the photochemistry of a realistic molecule (azobenzene) in strong coupling conditions, and characterization of an unexpected quantum yield enhanchement mechanism.
4. Applications of the models and software developed to specific case studies. Main results achieved along this line: Design of a nanoplasmonic setup to reveal quantum mechanical effects in a protein involved in the first stages of photosynthesis (i.e. in the harvesting of sun light); Simulation of existing ultrafast spectroscopy experiments using an atomistic, quantum mechanical description of the investigated molecules; Characterization at the atomistic level of how the mechanism of reactions induced by light are modified when molecules and plasmons both behave quantum mechanically and are hybridized.
