Novel molecular spectroscopies by nanoconfined light shaping and ab initio quantum dynamics

Description du projet

La spectroscopie moléculaire fait un grand bond en avant

En spectroscopie, forcer la lumière à passer dans des espaces ultraconfinés permet d’augmenter radicalement la résolution spatiale et temporelle. Le projet NanoLight-QD, financé par l’UE, est une collaboration interdisciplinaire visant à faire progresser les techniques de spectroscopie moléculaire de pointe. Ce projet effectuera des simulations informatiques ab initio pour observer et mieux comprendre les modes de vibration normaux d’une molécule ainsi que la dynamique des électrons dans les matériaux 2D. Pour confiner la lumière à l’échelle nanométrique, les chercheurs optimiseront la forme et la disposition des nanostructures plasmoniques à l’aide de l’intelligence artificielle. Cette dernière permettra d’augmenter la vitesse et la précision du calcul des densités d’électrons et de l’estimation de la façon dont la lumière circule autour des nanoparticules, opérations désormais effectuées sur la base de la théorie de la fonctionnelle de la densité et des équations de Maxwell.

Objectif

This is a project that explores the interface among nanooptics, nanomaterials and molecular spectroscopy. This project will be developed in collaboration with three top experimental groups at different research institutions, and will be carried out by Dr. Franco Bonafé under the supervision of Prof. Dr. Angel Rubio, Director of the Theory Department of MPSD.

The main goal of the project is to demonstrate that the spatial and temporal resolution of different spectroscopies can be improved by utilizing the ultra-strong confinement of structured light down to the nanoscale. To this purpose, we will optimize the shape and arrangement of plasmonic nanostructures using machine learning algorithms, combining real-time time-dependent density functional theory simulations coupled fully self-consistently to Maxwell's equations. The work is divided into three main parts with clear interdependent tasks and goals, namely: 1) geometry optimization of plasmonic nanostructures to enhance the confinement of light, and its application in photoelectron emission; 2) development of a frequency-domain linear-response technique to increase the resolution of tip-enhanced Raman spectra of molecular vibrations in nanocavities; and 3) study of near-field structured light for attosecond photoelectron spectra of 2D materials. Our predictions will be experimentally tested by our network of experimental groups.

Overall, the aim of the project is to push the limits of state-of-the-art molecular spectroscopy techniques by ab initio computer simulations, increasing our ability to understand the properties of matter both at the scales of molecular vibrations and of attosecond electron dynamics in 2D materials. The researcher will clearly benefit from gaining training in non-equilibrium ab initio methods and from the world-wide top level network of experimental collaborators, that will bring him to a new stage in his career towards becoming an independent group leader in theoretical spectroscopy.