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Cambridge University Press eBooks

Quantum Emitters

Lukáš Novotný, Bert Hecht

Published Oct 31, 2025• 0 citations
Publisher

Abstract

The chapter discusses quantum emitters, exploring their fundamental mechanisms, properties, and applications. Beginning with two-level systems, we introduce the concept of extinction cross-section. To capture phenomena, such as fluorescence, the discussion extends to four-level systems and spontaneous as well as stimulated emission processes, crucial for understanding laser operation. We then examine the dependence of the quantum yield on the local environment. Single-photon emission is scrutinized in terms of the second-order autocorrelation function through both steady-state and time-dependent analyses, providing a comprehensive understanding of this essential feature of quantum emitters. The chapter further addresses the generation of indistinguishable single photons, a key requirement for quantum computing and secure communication. Various types of quantum emitters are then introduced, including fluorescent molecules, semiconductor quantum dots, and color centers in diamond, each with unique properties and applications. Finally, single molecules are presented as probes for localized fields, with an in-depth look at field distributions in a laser focus and sources of strongly localized fields.

DOI
10.1017/9781108781503.010

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The chapter discusses quantum emitters, exploring their fundamental mechanisms, properties, and applications. Beginning with two-level systems, we introduce the concept of extinction cross-section. To capture phenomena, such as fluorescence, the discussion extends to four-level systems and spontaneous as well as stimulated emission processes, crucial for understanding laser operation. We then examine the dependence of the quantum yield on the local environment. Single-photon emission is scrutinized in terms of the second-order autocorrelation function through both steady-state and time-dependent analyses, providing a comprehensive understanding of this essential feature of quantum emitters. The chapter further addresses the generation of indistinguishable single photons, a key requirement for quantum computing and secure communication. Various types of quantum emitters are then introduced, including fluorescent molecules, semiconductor quantum dots, and color centers in diamond, each with unique properties and applications. Finally, single molecules are presented as probes for localized fields, with an in-depth look at field distributions in a laser focus and sources of strongly localized fields.
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The interaction of light with nanoscale structures is at the core of nano-optics. As the structures become smaller and smaller the laws of quantum mechanics will become apparent. In this limit, the discrete nature of atomic states gives rise to resonant light-matter interactions. In atoms, molecules, and nanoparticles, such as semiconductor nanocrystals and other “quantum confined” systems, these resonances occur when the photon energy matches the energy difference of discrete internal (electronic) energy levels. Owing to the resonant character, light-matter interaction can often be approximated by treating these quantum emitters as effective two-level systems, i.e. by considering only those two (electronic) levels whose difference in energy is close to the interacting photon energy ħω 0 . In this chapter we discuss quantum emitters that are used in optical experiments. We will discuss their use as single-photon sources and analyze their photon statistics. While the radiative properties of quantum emitters have been discussed in Chapter 8, this chapter focuses on the properties of the quantum emitters themselves. We adopt a rather practical perspective since more detailed accounts can be found elsewhere (see e.g. [1–4]). Types of quantum emitters The possibility of detecting single quantum emitters optically relies mostly on the fact that redshifted emission can be very efficiently discriminated against excitation light [5, 6]. This opens the road for experiments in which the properties of these emitters are studied or in which they are used as discrete light sources.
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.
LX centers are a recently discovered class of impurity centers in diamonds, which are characterized by nearly phononfree, spectral narrowband, and intense fluorescence at room temperature. Such a set of properties pave the way for a variety of applications, including sensing and single-photon emission. The latter requires a detailed study of photophysical processes of single emitters, which is the focus of this paper. The study of the luminescence dynamics of single LX centers in microdiamonds, synthesized by the high pressure-high temperature method, is performed by means of second-order cross-correlation function (g(2){g}^{(2)}g(2)) analysis. Even though the blinking is not observed directly in the measurements, the presence of photon bunching indicates that the fluorescence of a single emitter is intermittent at microsecond scale. The three-level system that is commonly used to describe intermittency of dye molecules is not consistent with the observed power dependences. We suggest a four-level energy system model with two metastable states to describe the results and perform numerical simulations to validate the model. Finally, we discuss the four-level model in the form of fluctuations of photophysical parameters.
A detailed study of the photophysical properties of several chromium-related color centers produced within chemical vapor deposition diamond is presented. These emitters show narrow luminescence lines in the range of $740\ensuremath{-}770$ nm. Single-photon emission was verified with continuous and pulsed excitation with detected emission rates at saturation in the range of ($2\ensuremath{-}3$) $\ifmmode\times\else\texttimes\fi{}$ 106{10}^{6}106 counts/s, while direct lifetime measurements reveal excited state lifetimes for the distinct centers ranging $1\ensuremath{-}14$ ns. In addition, a number of quantum emitters demonstrate two-level behavior with no bunching present in the second-order correlation function. The three-level systems revealed typically photoluminescence lines with width half-maximum of  4~4 4 nm while the two-level emitters have full width half-maximum of  10~10 10 nm at room temperature. In addition, the quantum efficiency of the two-level system was measured to be four times higher than that of the three-level system.