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arXiv:2102.13055

Indistinguishable photons on demand from an organic dye molecule

Pietro Lombardi, Maja Colautti, Rocco Duquennoy, Ghülam Murtaza, Prosenjit Majumder, Costanza Toninelli

Published Feb 25, 2021• 1 citation
arXivHTMLPDF

Abstract

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.

DOI
10.48550/arxiv.2102.13055

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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.
Scalability and miniaturization are hallmarks of solid-state platforms for photonic quantum technologies. Still a main challenge is two-photon interference from distinct emitters on chip. This requires local tuning, integration, and novel approaches to understand and tame noise processes. A promising platform is that of molecular single-photon sources. Thousands of molecules with optically tunable emission frequency can be easily isolated in solid matrices and triggered with pulsed excitation. We here discuss Hong–Ou–Mandel interference experiments using several couples of molecules within few tens of microns. Quantum interference is observed in real time, enabling the analysis of local environment effects at different time scales.
Scalability and miniaturization are hallmarks of solid-state platforms for photonic quantum technologies. Still a main challenge is two-photon interference from distinct emitters on chip. This requires local tuning, integration and novel approaches to understand and tame noise processes. A promising platform is that of molecular single photon sources. Thousands of molecules with optically tuneable emission frequency can be easily isolated in solid matrices and triggered with pulsed excitation. We here discuss Hong-Ou-Mandel interference experiments using several couples of molecules within few tens of microns. Quantum interference is observed in real time, enabling the analysis of local environment effects at different time-scales.