Photon emission correlation spectroscopy is an indispensable tool for the study of atoms, molecules, and, more recently, solid-state quantum defects. In solid-state systems, its most common use is as an indicator of single-photon emission, a key property for quantum technology. Beyond an emitter's single-photon purity, however, photon correlation measurements can provide a wealth of information that can reveal details about its electronic structure and optical dynamics that are hidden by other spectroscopy techniques. This tutorial presents a standardized framework for using photon emission correlation spectroscopy to study quantum emitters, including discussion of theoretical background, considerations for data acquisition and statistical analysis, and interpretation. We highlight important nuances and best practices regarding the commonly-used $g^{(2)}(\\tau=0)<0.5$ test for single-photon emission. Finally, we illustrate how this experimental technique can be paired with optical dynamics simulations to formulate an electronic model for unknown quantum emitters, enabling the design of quantum control protocols and assessment of their suitability for quantum information science applications.
Photon emission correlation spectroscopy is an indispensable tool for the study of atoms, molecules, and, more recently, solid-state quantum defects. In solid-state systems, its most common use is as an indicator of single-photon emission, a key property for quantum technology. Beyond an emitter's single-photon purity, however, photon correlation measurements can provide a wealth of information that can reveal details about its electronic structure and optical dynamics that are hidden by other spectroscopy techniques. This tutorial presents a standardized framework for using photon emission correlation spectroscopy to study quantum emitters, including discussion of theoretical background, considerations for data acquisition and statistical analysis, and interpretation. We highlight important nuances and best practices regarding the commonly-used g(2)(tau=0)<0.5 test for single-photon emission. Finally, we illustrate how this experimental technique can be paired with optical dynamics simulations to formulate an electronic model for unknown quantum emitters, enabling the design of quantum control protocols and assessment of their suitability for quantum information science applications.
Photon-emission-correlation spectroscopy is an indispensable tool for the study of atoms, molecules, and, more recently, solid-state quantum defects.In solid-state systems, its most common use is as an indicator of single-photon emission, a key property for quantum technology.Beyond the single-photon purity of an emitter, however, photon-correlation measurements can provide a wealth of information that can reveal details about its electronic structure and optical dynamics that are hidden by other spectroscopy techniques.This tutorial presents a standardized framework for using photon-emission-correlation spectroscopy to study quantum emitters, including discussion of theoretical background, considerations for data acquisition and statistical analysis, and interpretation.We highlight important nuances and best practices regarding the commonly used g (2) (τ = 0) < 0.5 test for single-photon emission.Finally, we illustrate how this experimental technique can be paired with optical-dynamics simulations to formulate an electronic model for unknown quantum emitters, enabling the design of quantum control protocols and assessment of their suitability for quantum information science applications.
Photon emission correlation spectroscopy (PECS) is an indispensable tool for the study of atoms, molecules, and, more recently, solid-state quantum defects. In solid-state systems, its most common use is as an indicator of single-photon emission, a key property for quantum technology. Beyond single-photon purity, photon correlation measurements can provide a wealth of information that can reveal details about an emitter's electronic structure and optical dynamics that are hidden by other spectroscopy techniques. This thesis explores the application of PECS to study and understand the optical dynamics of quantum emitters. The first part of this thesis presents a guide to a standardized framework for using PECS to facilitate materials exploration for qubit candidates. This includes discussion of theoretical background, considerations for data acquisition and statistical analysis, and interpretation of PECS. It also illustrates how this experimental technique can be paired with optical dynamics simulations to formulate an electronic model for unknown quantum emitters. The second part of this thesis implements the practices discussed in the first part to explore the optical dynamics of two systems: the nitrogen-vacancy (NV) center in diamond and a quantum emitter in hexagonal boron nitride (h-BN). The NV center is a promising platform for applications in quantum sensing, quantum communication, and quantum networks. In particular, its spin and charge dynamics constitute useful attributes that can be harnessed for quantum control protocols. This thesis models and quantifies the transition rates that govern spin and charge dynamics in the NV center, utilizing PECS measurements, analysis, and simulations as a function of magnetic field, and excitation power. These findings can further inform the design of quantum control protocols. H-BN hosts pure single-photon emitters that have shown evidence of optically detected electronic spin dynamics. However, the electrical and chemical structure of these optically addressable spins is unknown, and the nature of their spin-optical interactions remains mysterious. This thesis discusses time-domain optical and microwave experiments to characterize a single emitter in h-BN exhibiting room temperature optically detected magnetic resonance. It further discusses use of dynamical simulations to constrain and quantify transition rates in the model, and design of optical control protocols that optimize the signal-to-noise ratio for spin readout. This constitutes a necessary step towards quantum control of spin states in h-BN.
Emitters of single photons are essential resources for emerging quantum technologies and developed within different platforms including nonlinear optics and atomic and solid-state systems. The energy-level structures of emission processes are critical for reaching and controlling high-quality sources. The most commonly applied test uses a Hanbury Brown and Twiss (HBT) setup to determine the emitter energy-level structure based on fitting temporal correlations of photon detection events. However, only partial information about the emission process is extracted from such detection, that might be followed by an inconclusive fitting of the data. This process predetermines our limited ability to quantify and understand the dynamics in the photon emission process that are of importance for the applications in communication, sensing, and computing. In this work, we present a complete analysis based on all normalized coincidences between detection and no-detection events recorded in the same HBT setup to certify expected properties of an emitted photonic state. As a proof of concept we apply our methodology to single nitrogen-vacancy centers in diamond, in which case the certification conclusively rejects a model based on a two-level emitter that radiates a photonic state mixed with any classical noise background. Published by the American Physical Society 2024
Even though the quantized interaction between light and matter in the photoelectric effect is considered one of the cornerstones in the development of quantum mechanics, it was long thought impossible to directly observe the quantized nature of light itself. The advent of light-intensity autocorrelation techniques in the 1950s, first developed to study the size of stars, changed little in this perception, until true single-photon correlation spectroscopy from trapped ions was proven to be possible in the late 1970s: Photons from a single quantum emitter tend to arrive in bunches, but each light quantum is spaced apart in time—it is antibunched. Initially considered only as the workhorse of atomic quantum optics, over the past two decades, photon correlation techniques have become a standard in fields as diverse as quantum-information processing, biological imaging, polymer physics, and materials science, in general. The technique is particularly useful for probing materials that are specifically designed to emit or absorb light in optoelectronic devices, such as light-emitting diodes, solar cells, or lasers. The central question in such studies is how large a mesoscopic piece of material can become and still behave as an atom-like source of single photons. What interactions may arise between multiple excitations within a material, and what sort of dark states may give rise to intermittency in the stream of photons? We review the many different classes of optoelectronic materials for which photon-correlation spectroscopy has proven to offer useful insight into excited-state dynamics, ranging from molecular, over semiconductor to metallic nanostructures. The technique is particularly suited to probing mesoscopic aggregates of organic semiconductors since each single molecule acts as a quantum emitter itself.
Quantum emitters serve as essential on-demand photonic resources, generating quantum states of light such as single photons and entangled photon pairs while serving as interfaces between light and matter. Buried in the solid state, quantum emitters enable a straightforward adoption of advanced nanofabrication techniques, facilitating precise engineering of their photonic environment for scalable quantum technologies. In this review, we introduce the fundamentals of quantum emitters and the key metrics characterising their performance. We highlight three material platforms: quantum dots, defect centres in diamond, and defect centres in silicon carbide. We summarise the recent developments of these platforms and discuss their advancements in quantum applications, including quantum communication, computation, and sensing. Finally, we provide a comparison across the three platforms, along with an outlook on future directions and potential challenges.
The development of spectroscopic techniques able to detect and verify quantum coherence is a goal of increasing importance given the rapid progress of new quantum technologies, the advances in the field of quantum thermodynamics, and the emergence of new questions in chemistry and biology regarding the possible relevance of quantum coherence in biochemical processes. Ideally, these tools should be able to detect and verify the presence of quantum coherence in both the transient dynamics and the steady state of driven-dissipative systems, such as light-harvesting complexes driven by thermal photons in natural conditions. This requirement poses a challenge for standard laser spectroscopy methods. Here, we propose photon correlation measurements as a new tool to analyze quantum dynamics in molecular aggregates in driven-dissipative situations. We show that the photon correlation statistics of the light emitted in several models of molecular aggregates can signal the presence of coherent dynamics. Deviations from the counting statistics of independent emitters constitute a direct fingerprint of quantum coherence in the steady state. Furthermore, the analysis of frequency resolved photon correlations can signal the presence of coherent dynamics even in the absence of steady state coherence, providing direct spectroscopic access to the much sought-after site energies in molecular aggregates.