Room-temperature ultrafast nonlinear spectroscopy of a single molecule

Anno: 2018

Autori: Liebel M., Toninelli C., van Hulst NF.

Affiliazione autori: Barcelona Inst Sci & Technol, ICFO Inst Ciencies Foton, Barcelona, Spain; CNR, INO, Sesto Fiorentino, Italy; Univ Florence, LENS, I-50019 Sesto Fiorentino, Italy; ICREA, Pg Lluis Co 23, Barcelona, Spain.

Abstract: Single-molecule spectroscopy aims to unveil often hidden but potentially very important contributions of single entities to a system’s ensemble response. Albeit contributing tremendously to our ever growing understanding of molecular processes, the fundamental question of temporal evolution, or change, has thus far been inaccessible, thus painting a static picture of a dynamic world. Here, we finally resolve this dilemma by performing ultrafast time-resolved transient spectroscopy on a single molecule. By tracing the femtosecond evolution of excited electronic state spectra of single molecules over hundreds of nanometres of bandwidth at room temperature, we reveal their nonlinear ultrafast response in an effective three-pulse scheme with fluorescence detection. A first excitation pulse is followed by a phase-locked de-excitation pulse pair, providing spectral encoding with 25 fs temporal resolution. This experimental realization of true single-molecule transient spectroscopy demonstrates that two-dimensional electronic spectroscopy of single molecules is experimentally within reach.

Giornale/Rivista: NATURE PHOTONICS

Volume: 12 (1)      Da Pagina: 45  A: +

Maggiori informazioni: This research was funded by the European Commission (European Research Council (ERC) Advanced Grant 670949-LightNet), the Ministerio de Economia, Industria y Competitividad (MINECO) Severo Ochoa Programme for Centres of Excellence in R&D (SEV-2015-0522, FIS2015-69258-P, FIS2015-72409-EXP), the Catalan Agencia de Gestio dAjuts Universitaris i de Recerca (AGAUR; 2014SGR01540), Fundacio Privada Cellex and Generalitat de Catalunya through the CERCA programme. M.L. acknowledges financial support from the Marie-Curie International Fellowship, and co-funding of regional, national and international programmes (COFUND). C.T. thanks the COST Action Nanoscale Quantum Optics (MP1403) and acknowledges financial support from MIUR programme Q-Sec and Ente Cassa di Risparmio di Firenze (GRANCASSA). We thank A. Weigel and C. Schnedermann for helpful discussions while preparing the manuscript.
Parole chiavi: Excited states, Excited electronic state; Experimental realizations; Fluorescence detection; Single molecule spectroscopy; Temporal resolution; Transient spectroscopy; Two-dimensional electronic spectroscopies; Ultrafast nonlinear, Molecules
DOI: 10.1038/s41566-017-0056-5

Citazioni: 43
dati da “WEB OF SCIENCE” (of Thomson Reuters) aggiornati al: 2024-09-08
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