A Theoretical Chemistry Approach toA Theoretical Chemistry Approach to

TimeTime--Resolved Molecular Resolved Molecular PlasmonicsPlasmonics

TAMETAME--PlasmonsPlasmons

PI: Stefano Corni

HI: University of Padova

Partner: CNR-Nano, Modena

http://www.tame-plasmons.eu

ERC CoG 2015 - PE4:Physical and Analytical Chemical sciences

BackgroundBackground

• Real time atomic motion

by ultrafast spectroscopy

Ultrafast optics

However:• Spatial resolution limited by wavelength

• Ensemble measurements (blur details)

E.g., proteins of photosynthesis......

BackgroundBackground

• Real time atomic motion

by ultrafast spectroscopy

Ultrafast optics

However:• Spatial resolution limited by wavelength

• Ensemble measurements (blur details)

......

Add plasmonic nanoantenna• To focus light at the nanoscale

BUT: interpretation of results?

Localized Surface Plasmon

Au

tip

Ag

tip

E.g., proteins of photosynthesis

GoalGoal

To develop a Quantum Chemistry approach

to describe plasmon-enhanced

molecular optical processes in real time

ε(ω)

Maxwell eqns

⁞

Schrödinger eqn

TAMingTAMing PlasmonicPlasmonic ExperimentsExperiments

• Plasmon-enhanced High Harmonic GenerationExp: Kim et al. Nature 2008; Sivis et al. Nature 2012

• Sub-molecular STM electroluminescenceExp: Qiu et al. Science 2003

• Time-resolved SERSExp: Klingsporn et al.; Pozzi et al. JPCLett 2014

• Enhanced pump probe in multi-chromophoric system (e.g. light-harvesting proteins)Exp: not performed yet

Initial plan

The TeamThe Team

GiorgiaBrancolini

Gabriel

Gil

EmanueleCoccia

JacopoFregoni

...