Room-temperature ultrafast nonlinear spectroscopy of a single molecule

Year: 2018

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

Autors Affiliation: [Liebel, Matz; van Hulst, Niek F.] Barcelona Inst Sci & Technol, ICFO Inst Ciencies Foton, Barcelona, Spain.
[Toninelli, Costanza] CNR, INO, Sesto Fiorentino, Italy and Univ Florence, LENS, I-50019 Sesto Fiorentino, Italy.
[van Hulst, Niek F.] 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.


Volume: 12 (1)      Pages from: 45  to: 49

KeyWords: 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

Citations: 29
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