Single organic molecules for photonic quantum technologies

In the realm of fundamental quantum science and technologies, non-classical states of light, such as single-photon Fock states, are widely studied. However, current standards and metrological procedures are not optimized for low light levels. Progress in this crucial scientific domain depends on innovative metrology approaches, utilizing reliable devices based on quantum effects. We present a new generation of molecule-based single photon sources, combining their integration ...

Organic molecules have recently gained attention as novel sources of single photons. We present a joint experiment--theory analysis of the temperature-dependent emission spectra, zero-phonon linewidth, and second-order correlation function of light emitted from a single molecule. We observe spectra with a zero-phonon-line together with several additional sharp peaks, broad phonon sidebands, and a strongly temperature dependent homogeneous broadening. Our model includes both l...

Cooling atoms to ultralow temperatures has produced a wealth of opportunities in fundamental physics, precision metrology, and quantum science. The more recent application of sophisticated cooling techniques to molecules, which has been more challenging to implement due to the complexity of molecular structures, has now opened door to the longstanding goal of precisely controlling molecular internal and external degrees of freedom and the resulting interaction processes. This...

In the last decade, much theoretical research has focused on studying the strong coupling between organic molecules (or quantum emitters, in general) and light modes. The description and prediction of polaritonic phenomena emerging in this light-matter interaction regime have proven to be difficult tasks. The challenge originates from the enormous number of degrees of freedom that need to be taken into account, both in the organic molecules and in their photonic environment. ...

The on-chip integration of quantum light sources and nonlinear elements poses a serious challenge to the development of a scalable photonic platform for quantum information and communication. In this work we demonstrate the potential of a novel hybrid technology which combines single organic molecules as quantum emitters and dielectric chips, consisting of ridge waveguides and grating far-field couplers. Dibenzoterrylene molecules in thin anthracene crystals exhibit long-term...

The extraordinary success in laser cooling, trapping, and coherent manipulation of atoms has energized the efforts in extending this exquisite control to molecules. Not only are molecules ubiquitous in nature, but the control of their quantum states offers unparalleled access to fundamental constants and possible physics beyond the Standard Model. Quantum state manipulation of molecules can enable high-precision measurements including tests of fundamental symmetries and searc...

A single quantum emitter can possess a very strong intrinsic nonlinearity, but its overall promise for nonlinear effects is hampered by the challenge of efficient coupling to incident photons. Common nonlinear optical materials, on the other hand, are easy to couple to but are bulky, imposing a severe limitation on the miniaturization of photonic systems. In this work, we show that a single organic molecule acts as an extremely efficient nonlinear optical element in the stron...

While experiments with one or two quantum emitters have become routine in various laboratories, scalable platforms for efficient optical coupling of many quantum systems remain elusive. To address this issue, we report on chip-based systems made of one-dimensional subwavelength dielectric waveguides (nanoguides) and polycyclic aromatic hydrocarbon molecules. After discussing the design and fabrication requirements, we present data on coherent linear and nonlinear spectroscopy...

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 demonstrate two-photon interference using two remote single molecules as bright solid-state sources of indistinguishable photons. By varying the transition frequency and spectral width of one molecule, we tune and explore the effect of photon distinguishability. We discuss future improvements on the brightness of single-photon beams, their integration by large numbers on chips, and the extension of our experimental scheme to coupling and entanglement of distant molecules.