4 research outputs found
Indistinguishable Photons from a Single Molecule
We report the results of coincidence counting experiments at the output of a
Michelson interferometer using the zero-phonon-line emission of a single
molecule at . Under continuous wave excitation, we observe the absence
of coincidence counts as an indication of two-photon interference. This
corresponds to the observation of Hong-Ou-Mandel correlations and proves the
suitability of the zero-phonon-line emission of single molecules for
applications in linear optics quantum computation.Comment: To appear in Phys. Rev. Let
Spectroscopy of single phycoerythrocyanin monomers: dark state identification and observation of energy transfer heterogeneities.
Phycoerythrocyanin (PEC) is part of the light harvesting system of cyanobacteria. The PEC monomer contains one phycoviolobilin chromophore, which transfers excitation energy onto two phycocyanobilin chromophores. Many spectroscopical methods have been used in the past to study the bulk properties of PEC. These methods average over many molecules. Therefore, differences in the behavior of individual molecules remain hidden. The energy transfer within photosynthetic complexes is however sensitive to changes in the spectroscopic properties of the participating subunits. Knowledge about heterogeneities is therefore important for the description of the energy transfer in photosynthetic systems. Here, the recording of the fluorescence emission of single PEC molecules is used as a tool to obtain such information. Spectrally resolved detection as well as double resonance excitation of single PEC molecules is used to investigate their bleaching behavior. The trans isomer of the phycoviolobilin chromophore is identified as a short-lived dark state of monomeric PEC. Polarization sensitive single molecule detection is used for the direct observation of the energy transfer in individual PEC molecules. The experiments reveal that more than one-half of the PEC molecules exhibit an energy transfer behavior significantly different from the bulk. These heterogeneities persist on a time scale of several seconds. Model calculations lead to the conclusion that they are caused by minor shifts in the spectra of the chromophores