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Quantum Nanophotonic Materials, Devices, and Systems

Coherent molecular quantum photonics

Alex S. Clark

Published Oct 4, 2024• 0 citations
Publisher

Abstract

Single organic molecules make excellent single photon sources, emitting photons with high efficiency and at favourable wavelengths for coupling to other quantum systems, including alkali atoms. I will discuss techniques to create organic crystals containing single photon emitting molecules, and our recent results applying strain to these crystals to tune their emission wavelength. I will show that subsequent photons emitted by a single molecule can undergo quantum interference at a beam splitter, a vital tool in optical quantum computing and communication, and will discuss how discuss how to assess photon indistinguishability using both continuous and pulsed lasers. While molecular excitation and radiative emission is efficient, generated photons can be difficult to collect without the use of photonic structures. I will discuss our recent efforts in coupling single molecules to waveguides and nanophotonic cavities.

DOI
10.1117/12.3028752

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Single organic molecules make excellent single photon sources, emitting photons with high efficiency and at favourable wavelengths for coupling to other quantum systems, including alkali atoms. I will discuss techniques to create organic crystals containing single photon emitting molecules, and our recent results applying strain to these crystals to tune their emission wavelength. I will show that subsequent photons emitted by a single molecule can undergo quantum interference at a beam splitter, a vital tool in optical quantum computing and communication, and will discuss how discuss how to assess photon indistinguishability using both continuous and pulsed lasers. While molecular excitation and radiative emission is efficient, generated photons can be difficult to collect without the use of photonic structures. I will discuss our recent efforts in coupling single molecules to waveguides and nanophotonic cavities.
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.
Quantum light-matter interactions form the basis of many quantum technologies and much fundamental research. Organic molecules are an impressive platform for the generation of quantum light, both as single photon emitters and as collective systems. In this work, I investigate quantum light-matter interactions with molecules of dibenzoterrylene in crystals of anthracene. I outline methods to grow dibenzoterrylene-doped anthracene crystals, and I characterize the optical properties of cryogenically cooled molecules. I prepare collective systems composed of pairs of molecules interacting through their free-space electromagnetic fields. I demonstrate a method to tune interacting molecules into resonance to form superradiant and subradiant collective states. Finally, I present a platform for solid-state cavity QED based on molecules of dibenzoterrylene coupled to a nanophotonic cavity. This demonstration establishes a route toward scalable deterministic photon generation with molecules. I also tune pairs of cavity-coupled molecules into resonance to form distributed collective states, opening the door to cavity-mediated many-body interactions.
Developing reliable and efficient single-photon sources is crucial for advancing quantum technologies, relying on nonlinear frequency conversion or spontaneous emission from individual quantum emitters. While different types of single-photon sources excel in specific applications, none meet all criteria for an “ideal” source: exceptional brightness, high purity, and indistinguishability. To address this challenge, coupling single-photon emitters with designer nanostructures can significantly enhance emission performance, a pivotal area in quantum nanophotonics. This review summarizes recent advancements over the past decade in generating and manipulating single photons, emphasizing the pivotal role of nanostructure coupling. Single-photon emission systems—such as nonlinear crystals, solid-state defects, quantum dots, carbon nanotubes, and two-dimensional materials—are categorized quantitatively based on their ability to achieve high purity, indistinguishability, and brightness, presented in a three-dimensional technology map. Furthermore, nanostructure engineering is showcased for manipulating properties such as emission direction, polarization, chirality, and entanglement of single photons. By elucidating these critical aspects, this review aims to advance understanding of how advancements in nanostructured environments promise to shape the future of single-photon generation and manipulation within quantum nanophotonics.
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.
At cryogenic temperatures, organic single-photon sources (SPSs) offer Fourier-limited emission, virtually unlimited photostability, and emission wavelengths selectable by molecular design, making them attractive for quantum metrology, secure communication, and photonic quantum information processing. However, their efficient integration with photonic microstructures has remained challenging, limiting photon collection from single organic emitters under cryogenic operation. Here, we demonstrate a cryogenic planar metallo-dielectric antenna that efficiently directs the emission of a single dibenzoterrylene (DBT) molecule towards the collection optics. The device reaches a collection efficiency of 97% and delivers 100 million photons per second into the first lens. We measure a photon indistinguishability for the Fourier-limited transition of 91.2% while maintaining a high single-photon purity of 97.7% under strong continuous-wave (CW) and pulsed excitation. These results establish organic molecules as a high-performance platform for single-photon generation and represent an important step towards scalable organic quantum photonic technologies.