NanoLight-QD · Novel molecular spectroscopies by nanoconfined light shaping and ab initio quantum dynamics
Horizon 2020 — Marie Skłodowska-Curie Actions
- Duration
- 2020-04-01 → 2022-03-31
- EU contribution
- €162,806
- Participants
- 1
- Scheme
- MSCA-IF-EF-ST
Lines connect the coordinator with its partners.
Results in brief
Novel molecular spectroscopies by nanoconfined light shaping and ab initio quantum dynamics
The possibility to localize light below the diffraction limit, in particular by surface plasmons of metal nanostructures, already has a large number of applications in sensors, energy and catalysis, among other areas. Understanding the microscopic details and developing efficient computational tools that account for light-matter interactions at an atomistic level, including electronic, nuclear and photonic degrees of freedom in a fully self-consistent way, can unleash still unknown power of these system. This project aims to contribute to such a deep, microscopic understanding, by combining computational electrodynamics and quantum dynamics from first principle, to explore the confinement of electromagnetic fields down to the atomic scale. Due to the nature of plasmonic states, plasmon-induced processes are normally tackled either by solving Maxwell’s equations coupled to very approximate matter descriptions, or by looking only at the matter properties and prescribing electromagnetic fields. Bridging the gap between these two approaches is not an easy task due to the multiscale nature of these phenomea. We implemented methods to couple Maxwell’s equations with matter at different levels of approximation, and we applied them for three areas: 1) nanoscale generation of light with orbital angular momentum (OAM) in real space and real time; 2) light-driven spectroscopy and microscopy with sharp tips used in scanning tunneling microscopes (STM); 3) quantum point contact formation in 2D materials, namely WSe2. We implemented the different light-matter coupling methods in the free, open-source package Octopus, making use of its new multisystem framework that was developed alongside this project together with the Octopus team, which solves the dynamics for any number of arbitrary physical systems. For the Maxwell propagation we harnessed the Schrödinger form of Maxwell’s equations in Riemann-Silberstein representation, and for the matter systems we considered linear media as well as ab initio level within time-dependent density functional theory (TDDFT).
Data: CORDIS, © European Union
Project objective
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.
Original text from CORDIS.
Participants
- MAX-PLANCK-GESELLSCHAFT ZUR FORDERUNG DER WISSENSCHAFTEN EV · MUNCHENCoordinatorGermany
Links
Data: CORDIS, © European Union