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Photon statistics and dynamics of Fluorescence Resonance Energy Transfer

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 Added by Andrew J. Berglund
 Publication date 2002
  fields Physics
and research's language is English




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We report high time-resolution measurements of photon statistics from pairs of dye molecules coupled by fluorescence resonance energy transfer (FRET). In addition to quantum-optical photon antibunching, we observe photon bunching on a timescale of several nanoseconds. We show by numerical simulation that configuration fluctuations in the coupled fluorophore system could account for minor deviations of our data from predictions of basic Forster theory. With further characterization we believe that FRET photon statistics could provide a unique tool for studying DNA mechanics on timescales from 10^-9 to 10^-3 s.



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Motivated by recent experiments on photon statistics from individual dye pairs planted on biomolecules and coupled by fluorescence resonance energy transfer (FRET), we show here that the FRET dynamics can be modelled by Gaussian random processes with colored noise. Using Monte-Carlo numerical simulations, the photon intensity correlations from the FRET pairs are calculated, and are turned out to be very close to those observed in experiment. The proposed stochastic description of FRET is consistent with existing theories for microscopic dynamics of the biomolecule that carries the FRET coupled dye pairs.
Photonic quantum technologies call for scalable quantum light sources that can be integrated, while providing the end user with single and entangled photons on-demand. One promising candidate are strain free GaAs/AlGaAs quantum dots obtained by droplet etching. Such quantum dots exhibit ultra low multi-photon probability and an unprecedented degree of photon pair entanglement. However, different to commonly studied InGaAs/GaAs quantum dots obtained by the Stranski-Krastanow mode, photons with a near-unity indistinguishability from these quantum emitters have proven to be elusive so far. Here, we show on-demand generation of near-unity indistinguishable photons from these quantum emitters by exploring pulsed resonance fluorescence. Given the short intrinsic lifetime of excitons confined in the GaAs quantum dots, we show single photon indistinguishability with a raw visibility of $V_{raw}=(94.2pm5.2),%$, without the need for Purcell enhancement. Our results represent a milestone in the advance of GaAs quantum dots by demonstrating the final missing property standing in the way of using these emitters as a key component in quantum communication applications, e.g. as an entangled source for quantum repeater architectures.
We compute the resonance energy transfer (RET) in a system composed of two quantum emitters near a host dielectric matrix in which metallic inclusions are inserted until the medium undergoes a dielectric-metal transition at percolation. We show that there is no peak in the RET rate at percolation, in contrast to what happens with the spontaneous emission rate of an emitter near the same critical medium. This result suggests that RET does not strongly correlate with the local density of states.
We temporally resolve the resonance fluorescence from an electron spin confined to a single self-assembled quantum dot to measure directly the spins optical initialization and natural relaxation timescales. Our measurements demonstrate that spin initialization occurs on the order of microseconds in the Faraday configuration when a laser resonantly drives the quantum dot transition. We show that the mechanism mediating the optically induced spin-flip changes from electron-nuclei interaction to hole-mixing interaction at 0.6 Tesla external magnetic field. Spin relaxation measurements result in times on the order of milliseconds and suggest that a $B^{-5}$ magnetic field dependence, due to spin-orbit coupling, is sustained all the way down to 2.2 Tesla.
The electronic energy levels and optical transitions of a semiconductor quantum dot are subject to dynamics within the solid-state environment. In particular, fluctuating electric fields due to nearby charge traps or other quantum dots shift the transition frequencies via the Stark effect. The environment dynamics are mapped directly onto the fluorescence under resonant excitation and diminish the prospects of quantum dots as sources of indistinguishable photons in optical quantum computing. Here, we present an analysis of resonance fluorescence fluctuations based on photon counting statistics which captures the underlying time-averaged electric field fluctuations of the local environment. The measurement protocol avoids dynamic feedback on the electric environment and the dynamics of the quantum dots nuclear spin bath by virtue of its resonant nature and by keeping experimental control parameters such as excitation frequency and external fields constant throughout. The method introduced here is experimentally undemanding.
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