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arXiv:0707.3398 · Nature Physics

Efficient coupling of photons to a single molecule and the observation of its resonance fluorescence

G. Wrigge, Ilja Gerhardt, Jaesuk Hwang, G. Zumofen, Vahid Sandoghdar

Published Dec 16, 2007• 341 citations
arXivHTMLPDF
DOI
10.1038/nphys812

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Many of the currently pursued experiments in quantum optics would greatly benefit from a strong interaction between light and matter. Here, we present a simple new scheme for the efficient coupling of single molecules and photons. A glass capillary with a diameter of 600 nm filled with an organic crystal tightly guides the excitation light and provides a maximum spontaneous emission coupling factor (β) of 18% for the dye molecules doped in the organic crystal. A combination of extinction, fluorescence excitation, and resonance fluorescence spectroscopy with microscopy provides high-resolution spatiospectral access to a very large number of single molecules in a linear geometry. We discuss strategies for exploring a range of quantum-optical phenomena, including polaritonic interactions in a mesoscopic ensemble of molecules mediated by a single mode of propagating photons.
Intensity squeezing-i.e., photon number fluctuations below the shot-noise limit-is a fundamental aspect of quantum optics and has wide applications in quantum metrology. It was predicted in 1979 that intensity squeezing could be observed in resonance fluorescence from a two-level quantum system. However, its experimental observation in solid states was hindered by inefficiencies in generating, collecting, and detecting resonance fluorescence. Here, we report the intensity squeezing in a single-mode fiber-coupled resonance fluorescence single-photon source based on a quantum dot-micropillar system. We detect pulsed single-photon streams with 22.6% system efficiency, which show sub-shot-noise intensity fluctuation with an intensity squeezing of 0.59 dB. We estimate a corrected squeezing of 3.29 dB at the first lens. The observed intensity squeezing provides the last piece of the fundamental picture of resonance fluorescence, which can be used as a new standard for optical radiation and in scalable quantum metrology with indistinguishable single photons.