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A Theoretical Chemistry Approach to Time-Resolved Molecular Plasmonics TAME-Plasmons 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 Background Ultrafast optics • Real time atomic motion by ultrafast spectroscopy However: • Spatial resolution limited by wavelength • Ensemble measurements (blur details) ... ... E.g., proteins of photosynthesis Background Ultrafast optics Add plasmonic nanoantenna • Real time atomic motion by ultrafast spectroscopy • To focus light at the nanoscale Localized Surface Plasmon However: • Spatial resolution limited by wavelength • Ensemble measurements (blur details) ... ... E.g., proteins of photosynthesis Ag Au tip BUT: interpretation of results? Goal To develop a Quantum Chemistry approach to describe plasmon-enhanced molecular optical processes in real time Maxwell eqns ε(ω) ⁞ Schrödinger eqn TAMing Plasmonic Experiments Initial plan • Plasmon-enhanced High Harmonic Generation Exp: Kim et al. Nature 2008; Sivis et al. Nature 2012 • Sub-molecular STM electroluminescence Exp: Qiu et al. Science 2003 • Time-resolved SERS Exp: Klingsporn et al.; Pozzi et al. JPCLett 2014 • Enhanced pump probe in multi-chromophoric system (e.g. light-harvesting proteins) Exp: not performed yet The Team Giorgia Brancolini Emanuele Coccia Jacopo Fregoni Gabriel Gil ...