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Bulletin of the American Physical Society

Towards the coupling of single photons from dye molecules to a photonic waveguide

Claudio Polisseni, Kiang Wei Kho, Kyle D. Major, Samuele Grandi, Sebastien Boisser, Jaesuk Hwang, Alex S. Clark, Edward A. Hinds

Published Mar 18, 2016• 0 citations
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We point out that individual organic dye molecules, deposited close to optical waveguides on a photonic chip, can act as single-photon sources. A thin silicon nitride strip waveguide is expected to collect 28% of the photons from a single dibenzoterrylene molecule. These molecules can also provide large, localized optical nonlinearities, which are enough to discriminate between one photon or two through a differential phase shift of 2° per photon. This new atom–photon interface may be used as a resource for processing quantum information.

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Preparation and testing of organic dye molecules as single photon sources on a chip

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The physical realisation of a photonic quantum computer requires a reliable, fast, ondemand source of single indistinguishable photons. A promising candidate for one of these sources is a single dye molecule in a solid state matrix placed within the evanescent field of a photonic waveguide. This thesis explores the possibility of coupling of single dibenzoterrylene (DBT) molecules in an anthracene matrix to a silicon nitride waveguide at room temperature. I first discuss the theory by which photons from a DBT molecule can be evanescently coupled to a ridge waveguide. I present a novel growth method to form DBT-doped anthracene crystals which is very promising for applications to photonic devices. I discuss the methodology and the theory of such growth. I describe the confocal microscope I developed and used to image and characterise the emission of the single DBT molecules embedded in these crystals. My measurements show that the molecules are extremely stable single quantum emitters with a well-de ned polarization relative to the crystal axes. Measurements of the saturation intensity at room temperature allow me to estimate that a single DBT molecule could deliver at least 1012 photons before bleaching. This method of growth was used to deposit DBT molecules on top of a silicon nitride ridge waveguide. The results of the coupling experiment are shown. These include confocal images, saturation and lifetime measurements. The coupling efficiency is calculated and compared to what was simulated. The challenges of such structures are then presented. To tackle these challenges I deposited the molecules on top of lithium niobate and in silicon nitride slots. I conclude with a proposal for constructing the best photonic structure which would guarantee an easy deposition of the molecules and high coupling efficiencies.

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Single quantum emitters: resonance fluorescence and emission enhancement

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Single photons are highly desirable for encoding, sending and processing quantum information. Suitable engineering of single quantum emitters and their environment can lead to a reliable single photon source and to mediated photon-photon interactions, essential assets for quantum communication and computation purposes. Dye molecules, our chosen single quantum emitter, have attracted much attention in recent years due to their high photostability and narrow emission lines. In this thesis I present a detailed analysis of the optical properties of single dibenzoterrylene molecules in an anthracene matrix. Single photon emission is demonstrated at room and cryogenic temperatures. In the latter case, an analysis of the second-order correlation function of the emission of a single molecule is studied at various temperatures. The data agree with a full solution of the optical Bloch equations over a wide range of temperature, and provide some insight into the dephasing process of the molecules. I then present a technique for integrating single dye molecules with nano-photonic devices. These are hybrid plasmonic waveguides, designed to guide light and to enhance the interaction with a single emitter by a tight confinement of the waveguide mode. Single molecules are deposited over the waveguides and a first evidence of coupling is presented. I conclude with proposed improvements to the optical setup and to the deposition methods. Finally, I present another type of integrated device, where the light matter interaction is enhanced by inserting single quantum emitters into coupled optical resonators. The theoretical description for the case of resonant two-photon absorption from single atoms in coupled photonic crystal cavities is developed. I conclude by proposing a possible realisation of this system, and describing the first steps towards the fabrication of such a device.

•Apr 1, 2017•2 citations
We point out that individual organic dye molecules, deposited close to optical waveguides on a photonic chip, can act as single-photon sources. A thin silicon nitride strip waveguide is expected to collect 28% of the photons from a single dibenzoterrylene molecule. These molecules can also provide large, localized optical nonlinearities, which are enough to discriminate between one photon or two through a differential phase shift of 2° per photon. This new atom–photon interface may be used as a resource for processing quantum information.
The physical realisation of a photonic quantum computer requires a reliable, fast, ondemand source of single indistinguishable photons. A promising candidate for one of these sources is a single dye molecule in a solid state matrix placed within the evanescent field of a photonic waveguide. This thesis explores the possibility of coupling of single dibenzoterrylene (DBT) molecules in an anthracene matrix to a silicon nitride waveguide at room temperature. I first discuss the theory by which photons from a DBT molecule can be evanescently coupled to a ridge waveguide. I present a novel growth method to form DBT-doped anthracene crystals which is very promising for applications to photonic devices. I discuss the methodology and the theory of such growth. I describe the confocal microscope I developed and used to image and characterise the emission of the single DBT molecules embedded in these crystals. My measurements show that the molecules are extremely stable single quantum emitters with a well-de ned polarization relative to the crystal axes. Measurements of the saturation intensity at room temperature allow me to estimate that a single DBT molecule could deliver at least 1012 photons before bleaching. This method of growth was used to deposit DBT molecules on top of a silicon nitride ridge waveguide. The results of the coupling experiment are shown. These include confocal images, saturation and lifetime measurements. The coupling efficiency is calculated and compared to what was simulated. The challenges of such structures are then presented. To tackle these challenges I deposited the molecules on top of lithium niobate and in silicon nitride slots. I conclude with a proposal for constructing the best photonic structure which would guarantee an easy deposition of the molecules and high coupling efficiencies.
Single photons are highly desirable for encoding, sending and processing quantum information. Suitable engineering of single quantum emitters and their environment can lead to a reliable single photon source and to mediated photon-photon interactions, essential assets for quantum communication and computation purposes. Dye molecules, our chosen single quantum emitter, have attracted much attention in recent years due to their high photostability and narrow emission lines. In this thesis I present a detailed analysis of the optical properties of single dibenzoterrylene molecules in an anthracene matrix. Single photon emission is demonstrated at room and cryogenic temperatures. In the latter case, an analysis of the second-order correlation function of the emission of a single molecule is studied at various temperatures. The data agree with a full solution of the optical Bloch equations over a wide range of temperature, and provide some insight into the dephasing process of the molecules. I then present a technique for integrating single dye molecules with nano-photonic devices. These are hybrid plasmonic waveguides, designed to guide light and to enhance the interaction with a single emitter by a tight confinement of the waveguide mode. Single molecules are deposited over the waveguides and a first evidence of coupling is presented. I conclude with proposed improvements to the optical setup and to the deposition methods. Finally, I present another type of integrated device, where the light matter interaction is enhanced by inserting single quantum emitters into coupled optical resonators. The theoretical description for the case of resonant two-photon absorption from single atoms in coupled photonic crystal cavities is developed. I conclude by proposing a possible realisation of this system, and describing the first steps towards the fabrication of such a device.