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

By G. Wrigge, I. Gerhardt, Jaesuk Hwang, G. Zumofen, Vahid Sandoghdar. 2007

302 citations recorded by the source corpus.

Single dye molecules at cryogenic temperatures exhibit many spectroscopic phenomena known from the study of free atoms and are thus promising candidates for experiments in fundamental quantum optics. However, the existing techniques for their detection have either sacrificed information on the coherence of the excited state or have been inefficient. Here, we show that these problems can be addressed by focusing the excitation light near to the extinction cross-section of a molecule. Our detection scheme enables us to explore resonance fluorescence over nine orders of magnitude of excitation intensity and to separate its coherent and incoherent parts. In the strong excitation regime, we demonstrate the first direct observation of the Mollow fluorescence triplet from a single solid-state emitter. Under weak excitation, we report the detection of a single molecule with an incident power as faint as 600 aW, paving the way for studying nonlinear effects with only a few photons.

Subfields: Artificial Intelligence, Atomic and Molecular Physics, and Optics, Biomedical Engineering

View Paper: https://www.semanticscholar.org/paper/b6cfe77284cab4485b560a213fe29264b2cc3800

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Citations in the corpus

Spin-resolved quantum-dot resonance fluorescence (2008, background): “It was first observed on atomic sodium [33] in 1975 and more recently on a single molecule [34], but with little prospect of linkage to any spin states.”
Resonantly driven coherent oscillations in a solid-state quantum emitter (2009, background): “Coherent control with simultaneous generation of photons has been an elusive goal in solid-state approaches, where, because of strong laser scattering at the detection wavelength, measurement of resonant emission has been limited to cross-polarized detectio”
Cavity QED with atomic mirrors (2012, background): “Thus far, the available techniques to efficiently couple single photons with atomic media fall into one of the following, mostly independent, categories: i) cavity quantum electrodynamics (QED) [3–5], where atomic interactions with light are enhanced via a high-finesse cavity, ii) coherent coupling ”
Cavity-based quantum networks with single atoms and optical photons (2014, background): “Clearly, this condition is not achievable in free space, even when using tight but diffraction limited focusing of a Gaussian input mode (van Enk and Kimble, 2000; Tey et al., 2008; Wrigge et al., 2008).”
Non-resonant dot–cavity coupling and its potential for resonant single-quantum-dot spectroscopy (2009, unknown): “[28] Wrigge, G.”
Femtosecond coherence and quantum control of single molecules at room temperature (2010, background): “In the coherent regime we are able to induce Rabi oscillations, which was on single systems so far only observed on organic molecules in crystalline matrice”