Fluorescence-detected two-dimensional electronic spectroscopy of a single molecule

Abstract

Single-molecule fluorescence spectroscopy is a powerful method that avoids ensemble averaging, but its temporal resolution is limited by the fluorescence lifetime to nanoseconds at most. At the ensemble level, two-dimensional spectroscopy provides insight into ultrafast femtosecond processes such as energy transfer and line broadening, even beyond the Fourier limit, by correlating pump and probe spectra. Here, we combine these two techniques and demonstrate 2D spectroscopy of individual molecules at room temperature using the example of dibenzoterrylene (DBT) in a polymer matrix. We excite the molecule in a confocal microscope with a phase-modulated train of femtosecond pulses and detect the emitted fluorescence with single-photon counting detectors. Using a phase sensitive detection scheme, we were able to measure the nonlinear 2D spectra of most of the DBT molecules we studied. Our method is applicable to a wide range of single emitters and opens new avenues for understanding energy transfer in single quantum objects on ultrafast time scales.

10 pages, 4 figures

References in corpus (8)

• Spatially-resolved Fluorescence-detected Two-dimensional Electronic Spectroscopy Probes Varying Electronic Couplings in Photosynthetic Bacteria
• Room-temperature ultrafast non-linear spectroscopy of a single molecule
• Near-infrared single-photons from aligned molecules in ultrathin crystalline films at room temperature
• Ultrafast Energy Relaxation in Single Light-Harvesting Complexes
• Plasmon mediated coherent population oscillations in molecular aggregates
• Phase-Modulated Rapid-Scanning Fluorescence-Detected Two-Dimensional Electronic Spectroscopy
• Single Molecule Nonlinearity in a Plasmonic Waveguide
• Compressed Sensing for Reconstructing Coherent Multidimensional Spectra

Cited by in corpus (4)

• Influence of excitonic coupling, static disorder, and coherent dynamics in action-2D electronic spectroscopy of a molecular dimer model
• Overcoming experimental obstacles in two-dimensional spectroscopy of a single molecule
• Disentangling Single- and Biexciton Dynamics with Photoelectron-Detected Two-Dimensional Electronic Spectroscopy
• Low-dispersive phase-modulated rapid scanning interferometry