Nonclassical Photon Statistics in Single-Molecule Fluorescence at Room Temperature

Fleury, L.; Segura, Jean-Manuel; Zumofen, G.; Hecht, Bert; Wild, Urs P.

doi:10.1103/physrevlett.84.1148

Cited by 233 publications

(231 citation statements)

References 23 publications

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“…However, this hypothesis is contradicted to previous reports, which revealed shortened off-states due to the high pumping power. [32][33][34] Additionally, the examination of time traces from the dye immobilized monolayer on SIF with higher excitation power completely eliminates this hypothesis, as the time profiles provided no evidence that the blinking is dependent on the excitation intensity on silvered surfaces (data not shown).…”

Section: Fluorescence Time Tracesmentioning

confidence: 99%

Enhanced Fluorescence of Cy5-Labeled Oligonucleotides Near Silver Island Films: A Distance Effect Study Using Single Molecule Spectroscopy

Lakowicz

2006

J. Phys. Chem. B

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We investigated fluorescence enhancements and lifetime reductions of Cy5 probe molecules at various distances from the deposited silver island film surface using single molecule spectroscopic methods. The proximity of fluorophore molecules to the surface was controlled by alternating layers of biotinylated bovine serum albumin (BSA-biotin) and avidin, followed by binding of Cy5-labeled oligonucleotides to the top of a BSA-biotin layer structure. We observed dramatically varied brightness of fluorophores with distances from metal structures as well with reduced blinking in the presence of silver island films. In addition, distributions of fluorescence lifetimes and apparent emission intensities from individual molecules indicate an inhomogeneous nature of local matrix surface near metallic nanostructures. These studies illustrate the exclusive information that is otherwise hidden in ensemble measurements.

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Section: Fluorescence Time Tracesmentioning

confidence: 99%

Enhanced Fluorescence of Cy5-Labeled Oligonucleotides Near Silver Island Films: A Distance Effect Study Using Single Molecule Spectroscopy

Lakowicz

2006

J. Phys. Chem. B

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“…A few other studies have touched on specific aspects of quantum dynamics applicable to SMS [24,27,[33][34][35], but without complete generality. Recent work by us [36][37][38][39] and others [40][41][42][43][44],has established generating function techniques as a general means for calculating statistical quantities of single molecule photon counting experiments.…”

Section: Introductionmentioning

confidence: 99%

Single Molecule Photon Counting Statistics for Quantum Mechanical Chromophore Dynamics

2006

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We extend the generating function technique for calculation of single molecule photon emission statistics [Y. Zheng and F. L. H. Brown, Phys. Rev. Lett., 90,238305 (2003)] to systems governed by multi-level quantum dynamics. This opens up the possibility to study phenomena that are outside the realm of purely stochastic and mixed quantum-stochastic models. In particular, the present methodology allows for calculation of photon statistics that are spectrally resolved and subject to quantum coherence. Several model calculations illustrate the generality of the technique and highlight quantitative and qualitative differences between quantum mechanical models and related stochastic approximations. Calculations suggest that studying photon statistics as a function of photon frequency has the potential to reveal more about system dynamics than the usual broadband detection schemes.

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“…Temporally and spectrally resolved measurements can reveal important matter information. Recent single photon spectroscopy of single molecules (Fleury et al, 2000;Lettow et al, 2010;Rezus et al, 2012) call for an adequate microscopic foundation where joint matter and field information could be retrieved by a proper description of the detection process. A microscopic diagrammatic approach may be used for calculating time-and-frequency gated photon counting measurements (Dorfman and Mukamel, 2012a).…”

Section: Multiple Photon Counting Detectionmentioning

confidence: 99%

Nonlinear optical signals and spectroscopy with quantum light

2016

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Conventional nonlinear spectroscopy uses classical light to detect matter properties through the variation of its response with frequencies or time delays. Quantum light opens up new avenues for spectroscopy by utilizing parameters of the quantum state of light as novel control knobs and through the variation of photon statistics by coupling to matter. We present an intuitive diagrammatic approach for calculating ultrafast spectroscopy signals induced by quantum light, focusing on applications involving entangled photons with nonclassical bandwidth properties -known as "time-energy entanglement". Nonlinear optical signals induced by quantized light fields are expressed using time ordered multipoint correlation functions of superoperators in the joint field plus matter phase space. These are distinct from Glauber's photon counting formalism which use normally ordered products of ordinary operators in the field space. One notable advantage for spectroscopy applications is that entangled photon pairs are not subjected to the classical Fourier limitations on the joint temporal and spectral resolution. After a brief survey of properties of entangled photon pairs relevant to their spectroscopic applications, different optical signals, and photon counting setups are discussed and illustrated for simple multi-level model systems.

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Nonclassical Photon Statistics in Single-Molecule Fluorescence at Room Temperature

Cited by 233 publications

References 23 publications

Enhanced Fluorescence of Cy5-Labeled Oligonucleotides Near Silver Island Films: A Distance Effect Study Using Single Molecule Spectroscopy

Enhanced Fluorescence of Cy5-Labeled Oligonucleotides Near Silver Island Films: A Distance Effect Study Using Single Molecule Spectroscopy

Single Molecule Photon Counting Statistics for Quantum Mechanical Chromophore Dynamics

Nonlinear optical signals and spectroscopy with quantum light

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