Molecules as Sources for Indistinguishable Single Photons

The advent of single molecule optics has had a profound impact in fields ranging from biophysics to material science, photophysics, and quantum optics. However, all existing room-temperature single molecule methods have been based on fluorescence detection of highly efficient emitters. Here we demonstrate that standard, modulation-free measurements known from conventional absorption spectrometers can indeed detect single molecules. We report on quantitative measurements of th...

A scanning tunneling microscope (STM) can do more than atomic imaging and manipulation. Its tunneling current can also be used for the excitation of light, converting electron energy to photon energy. STM based single-molecule electroluminescence can be realized by adopting a combined strategy of both efficient electronic decoupling and nanocavity plasmonic enhancement. The emission intensity, upon optimized material combination for the molecule, spacer, tip, and substrate, c...

Using the zero-phonon line (ZPL) emission of a single molecule, we realized a triggered source of near-infra-red (lambda=785 nm) single photons at a high repetition rate. A Weierstrass solid immersion lens is used to image single molecules with an optical resolution of 300 nm (~0.4*lambda) and a high collection efficiency. Because dephasing of the transition dipole due to phonons vanishes at liquid helium temperatures, our source is attractive for the efficient generation of ...

We report on the excitation of single molecules via narrow zero-phonon transitions using short laser pulses. By monitoring the Stokes-shifted fluorescence, we studied the excited state population as a function of the delay time, laser intensity, and frequency detuning. A pi-pulse excitation was demonstrated with merely 500 photons, and 5 Rabi cycles were achieved at higher excitation powers. Our findings are in good agreement with theoretical calculations and provide a first ...

The small cross section of Raman scattering poses a great challenge for its direct study at the single-molecule level. By exploiting the high Franck-Condon factor of a common-mode resonance, choosing a large vibrational frequency difference in electronic ground and excited states and operation at T < 2K, we succeed at driving a coherent stimulated Raman transition in individual molecules. We observe and model a spectral splitting that serves as a characteristic signature of t...

An array of radiatively coupled emitters is an exciting new platform for generating, storing, and manipulating quantum light. However, the simultaneous positioning and tuning of multiple lifetime-limited emitters into resonance remains a significant challenge. Here we report the creation of superradiant and subradiant entangled states in pairs of lifetime-limited and sub-wavelength spaced organic molecules by permanently shifting them into resonance with laser-induced tuning....

We point out that individual organic dye molecules, deposited close to optical waveguides on a photonic chip, can act as single photon sources and can also provide localised, giant optical nonlinearities. This new atom-photon interface may be used as a resource for processing quantum information.

We study the influence of a scanning nano-electrode on fluorescence excitation spectra of single terrylene molecules embedded in thin p-terphenyl films at cryogenic temperatures. We show that applied voltages less than 10 V can result in reversible Stark shifts of up to 100 times and linewidth increase greater than 10 times the natural linewidth. We discuss the potential of our experimental scheme for direct imaging of individual two-level systems (TLS) in the nanometer vicin...

Quantum technologies are the next big revolution in information technologies, computing, communication security, sensing as well as metrology. What do you use to explore all these fascinating applications when you work in Optics? Photons of course. In this review, we discuss the different available single photon source technologies, compare and contrast them in terms of applicability and properties, discuss state of the art and conclude that the future is indeed bright!

The electronic excitation of molecules triggers diverse phenomena such as luminescence and photovoltaic effects, which are the bases of various energy-converting devices. Understanding and control of the excitations at the single-molecule level are long standing targets, however, they have been hampered by the limited spatial resolution in optical probing techniques. Here we investigate the electronic excitation of a single molecule with sub-molecular precision using a locali...