ArticleThe journal of physical chemistry letters2015
Shaped and Feedback-Controlled Excitation of Single Molecules in the Weak-Field Limit.
Article in The journal of physical chemistry letters, 2015. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 6 papers.
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Who cites it
6 citing papers in PubMed.
- Single-molecule excitation-emission spectroscopy.Proceedings of the National Academy of Sciences of the United States of America · 2019Article
- Monitoring of Nonadiabatic Effects in Individual Chromophores by Femtosecond Double-Pump Single-Molecule Spectroscopy: A Model Study.Molecules (Basel, Switzerland) · 2019Article
- Rapid and robust control of single quantum dots.Light, science & applications · 2017Article
- Sub-10 fs Time-Resolved Vibronic Optical Microscopy.The journal of physical chemistry letters · 2016Article
- Proposal for probing energy transfer pathway by single-molecule pump-dump experiment.Scientific reports · 2016Article
- Broadband single-molecule excitation spectroscopy.Nature communications · 2016Article
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Authors and funding
3 authors.
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No grant is acknowledged in the PubMed record.
Abstract
Coherent control uses tailored femtosecond pulse shapes to influence quantum pathways and drive a light-induced process toward a specific outcome. There has been a long-standing debate whether the absorption properties or the probability for population to remain in an excited state of a molecule can be influenced by the pulse shape, even if only a single photon is absorbed. Most such experiments are performed on many molecules simultaneously, so that ensemble averaging reduces the access to quantum effects. Here, we demonstrate systematic coherent control experiments on the fluorescence intensity of a single molecule in the weak-field limit. We demonstrate that a delay scan of interfering pulses reproduces the excitation spectrum of the molecule upon Fourier transformation, but that the spectral phase of a pulse sequence does not affect the transition probability. We generalize this result to arbitrary pulse shapes by performing the first closed-loop coherent control experiments on a single molecule.
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