july, 2021

21jul15:0016:00FeaturedVirtual EventAttoChem webinar (E. Coccia)Role of coherence in ultrafast spectroscopy on single molecules and nanostructures

Event Details

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 [2]. 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 [4], 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 [2]. 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 [4] and vibrational [5] 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 [6]: 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.

[1] E. Collini, Chem. Soc. Rev. 2013, 42, 4932
[2] D. Brinks, R. Hildner, E. M. H. P. van Dijk, F. D. Stefani, J. B. Nieder and N. F. van Hulst. Chem. Soc. Rev. 2014, 43, 2476
[3] E. Coccia and S. Corni, J. Chem. Phys. 2019, 151, 044703
[4] E. Coccia, F. Troiani and S. Corni, J. Chem. Phys. 2018, 148, 204112
[5] G. Dall’Osto, E. Coccia, C. Guido and S. Corni, Phys. Chem. Chem. Phys. 2020, 22, 16734
[6] E. Coccia, J. Fregoni, CA Guido, M. Marsili, S. Pipolo, S. Corni, J. Chem. Phys. 2020, 153,

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(Wednesday) 15:00 - 16:00


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