Emanuele Coccia, University Of Trieste, IT.“Role of coherence in ultrafast spectroscopy on single molecules and nanostructures”Chair: Alessandra Ciavardini (University Of Nova Gorica – ELETTRA, EU)
Emanuele Coccia, University Of Trieste, IT.
“Role of coherence in ultrafast spectroscopy on single molecules and nanostructures”
Chair: Alessandra Ciavardini (University Of Nova Gorica – ELETTRA, EU)
Abstract: Ultrafast spectroscopy is a powerful tool to investigate, control and manipulate quantumcoherence in molecules and complex systems [1-2]. Detection of electronic and vibrational coherence in biological systems and in plasmonic nanostructures is a matter of stimulating and open debate [2-3]. Recently, specific ultrafast spectroscopy techniques could probe a single molecule . To understand the outcomes of such experiments, theoretical and computational approaches are required, able to include all the important features of the simulated system. Using a recently developed computational approach coupling the theory of open quantum systems, by means of stochastic Schrödinger equation , with a quantum-chemical description of the molecular target, we have simulated a two-pulse experiment on the TDI and DNQDI fluorophores [4-5], both investigated experimentally . We study which kind of information can be inferred from the evolution of the TDI and DNQDI fluorescence as a function of the delay time and phase shift between the two pulses. A complete rationalization of the experiments has been carried out, leading to a clear description of the appearance of electronic  and vibrational  coherence in a twopulse spectroscopy on single molecule. Moreover, we show that electronic decoherence can be thought as a further design element in molecular nanoplasmonics : metal nanoparticle effects on the absorption of light by a nearby molecule may be strongly affected (even qualitatively, i.e., suppression vs enhancement) by molecular decoherence.
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