Journal
NATURE PHOTONICS
Volume 12, Issue 1, Pages 45-+Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41566-017-0056-5
Keywords
-
Categories
Funding
- European Commission (European Research Council (ERC) [670949-LightNet]
- Ministerio de Economia, Industria y Competitividad (MINECO) Severo Ochoa Programme for Centres of Excellence in RD [SEV-2015-0522, FIS2015-69258-P, FIS2015-72409-EXP]
- Catalan Agencia de Gestio dAjuts Universitaris i de Recerca (AGAUR) [2014SGR01540]
- Fundacio Privada Cellex
- Marie-Curie International Fellowship
- COST Action Nanoscale Quantum Optics [MP1403]
- Ente Cassa di Risparmio di Firenze (GRANCASSA)
- Generalitat de Catalunya through the CERCA programme
- MIUR programme Q-Sec
- regional, national and international programmes (COFUND)
Ask authors/readers for more resources
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.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available