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Quantum Information and Measurement (QIM)

Organic Dye Molecules as Single Photon Sources for Optical Quantum Technologies

Pietro Lombardi, R. Emadi, Rocco Duquennoy, Ghiilam Murtaza, Maja Colautti, Costanza Toninelli

Published Jan 1, 2021• 1 citation
Publisher

Abstract

We present Hong-Ou-Mandel (HOM) experiments with photons emitted by a single molecule of Dibenzoterrylene in an Anthracene nanocrystal under pulsed excitation, and preliminary results for photons emitted by two spatially-separated molecules on the same sample.
DOI
10.1364/qim.2021.tu2b.3

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Single molecules in solid-state matrices have been proposed as sources of single-photon Fock states back 20 years ago. Their success in quantum optics and in many other research fields stems from the simple recipes used in the preparation of samples, with hundreds of nominally identical and isolated molecules. Main challenges as of today for their application in photonic quantum technologies are the optimization of light extraction and the on-demand emission of indistinguishable photons. We here present Hong-Ou-Mandel experiments with photons emitted by a single molecule of dibenzoterrylene in an anthracene nanocrystal at 3 K, under continuous wave and also pulsed excitation. A detailed theoretical model is applied, which relies on independent measurements for most experimental parameters, hence allowing for an analysis of the different contributions to the two-photon interference visibility, from residual dephasing to spectral filtering.
Single molecules in solid state matrices have been proposed as sources of single photon Fock states back 20 years ago. Their success in quantum optics and in many other research fields stems from the simple recipes used in the preparation of samples, with hundreds of nominally identical and isolated molecules. Main challenges as of today for their application in photonic quantum technologies are the optimization of light extraction and the on-demand emission of indistinguishable photons. We here present Hong–Ou–Mandel (HOM) experiments with photons emitted by a single molecule of dibenzoterrylene in an anthracene nanocrystal at 3 K, under continuous wave and also pulsed excitation. A detailed theoretical model is applied, which relies on independent measurements for most experimental parameters, hence allowing for an analysis of the different contributions to the two-photon interference visibility, from residual dephasing to spectral filtering. A HOM interference visibility of more than 75% is reported, which, according to the model, is limited by the residual dephasing present at the operating temperature.
Quantum light sources are crucial for the future of quantum photonic technologies and, among them, single photons on-demand are key resources in quantum communications and information processing. Ideal quantum emitters providing indistinguishable photons in a clocked manner, negligible decoherence and spectral diffusion, and with potential for scalability are today still a major challenge. We report on photostable and indistinguishable single photon emission from dibenzoterrylene molecules isolated in anthracene nanocrystals (DBT:Ac NCs) at 3K. The visibility of two-photon interference is preserved even when they are separated more than thirty times the excited-state lifetime, or ten fluorescence cycles. One of the advantages of organic molecules is the low-cost mass production of nominally identical emitters, that also allow for on-chip integration. These aspects combined with high spectral stability and coherence make them promising for applications and future quantum technologies.
The generation of non-classical light, especially of single photon states, is mostly limited to non-linear optics in crystals and single emitters. Here we perform research on single organic dye molecules under cryogenic conditions. The molecules are well-behaved and do not blink or bleach. Also they exhibit an enormous brightness (>106 detected counts per second) and have narrow-band emission (<15-20MHz). By atomic sodium vapor we are able to suppress unwanted background emission from residual impurities in the sample. This light is now analyzed for the use in all-optical gates and further quantum optical schemes. A first step is the characterization in a Hong-Ou-Mandel type experiment. Different variations of this are possible – reaching from indistinguishable to distinguishable photons impinging on a beam-splitter.
Single organic molecules hold great promise for generating, manipulating, and storing single photons. Such processes form the basis for new quantum-enhanced technologies such as sensing, communications, and computation. In this talk I will focus on a particularly promising molecule – dibenzoterrylene (DBT). When DBT is introduced into a solid crystal of anthracene it is photostable and emits light between 780 and 795 nm. When cooled to cryogenic temperature, DBT is isolated from phonon-induced dephasing meaning that the photons have a lifetime-limited. I will present recent results in growing DBT-doped anthracene crystals, introducing these to nanophotonic interfaces for enhancing the collection of photons, tuning the DBT emission wavelength to coincide with rubidium atomic absorption, and finally pump-probe spectroscopy experiments to find long-lived triplet states in DBT which will be useful for building a single-molecule quantum memory.
A reliable single photon source is required for many aspects of quantum technology. Organic molecules are attractive for this application because they can have high quantum yield and can be photostable, even at room temperature. To generate a photon with high probability, a laser must excite the molecule efficiently. We develop a simple model for that efficiency and discuss how to optimise it. We demonstrate the validity of our model through experiments on a single dibenzoterrylene (DBT) molecule in an anthracene crystal. We show that the excitation probability cannot exceed 75% at room temperature, but can increase to over 99% if the sample is cooled to liquid nitrogen temperature. The possibility of high photon generation efficiency with only modest cooling is a significant step towards a reliable photon source that is simple and practical.