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

ended

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.