Aluminum nitride is a technologically important wide band-gap semiconductor which has been shown to host bright quantum emitters. We use photon emission correlation spectroscopy (PECS), time-resolved photoluminescence (TRPL), and state-population dynamic simulations to probe the dynamics of emission under continuous wave (CW) and pulsed optical excitation. We infer that there are at least four dark shelving states, which govern the TRPL, bunching, and saturation of the optical transition. We study in detail the emission dynamics of two quantum emitters (QEs) with differing power-dependent shelving processes, hypothesized to result from charge ionization and recombination. These results demonstrate that photon bunching caused by shelving the system in a dark state inherently limits the saturation rate of the photon source. In emitters where increasing optical power deshelves the dark states, we observe an increased photon emission intensity. Published by the American Physical Society 2024
Aluminum nitride is a technologically important wide band-gap semiconductor which has been shown to host bright quantum emitters. We use photon emission correlation spectroscopy (PECS), time-resolved photoluminescence (TRPL), and state-population dynamic simulations to probe the dynamics of emission under continuous wave (CW) and pulsed optical excitation. We infer that there are at least four dark shelving states, which govern the TRPL, bunching, and saturation of the optical transition. We study in detail the emission dynamics of two quantum emitters (QEs) with differing power-dependent shelving processes, hypothesized to result from charge ionization and recombination. These results demonstrate that photon bunching caused by shelving the system in a dark state inherently limits the saturation rate of the photon source. In emitters where increasing optical power deshelves the dark states, we observe an increased photon emission intensity. Published by the American Physical Society 2024
Aluminum nitride is a technologically important wide bandgap semiconductor which has been shown to host bright quantum emitters. In this paper, we probe the photodynamics of quantum emitters in aluminum nitride using photon emission correlations and time-resolved spectroscopy. We identify that each emitter contains as many as 6 internal energy levels with distinct laser power-dependent behaviors. Power-dependent shelving and de-shelving processes, such as optically induced ionization and recombination are considered, indicating complex optical dynamics associated with the spontaneous and optically pumped transitions. State population dynamics simulations qualitatively explain the temporal behaviours of the quantum emitters, revealing that those with pump-dependent de-shelving processes can saturate at significantly higher intensities, resulting in bright room-temperature quantum light emission.
Solid-state quantum emitters (QEs) are fundamental in photonic-based quantum information processing. There is strong interest to develop high-quality QEs in III-nitride semiconductors because of their sophisticated manufacturing driven by large and growing applications in optoelectronics, high voltage power transistors, and microwave amplifiers. Here, the generation and direct integration of QEs in an aluminum nitride-based photonic integrated circuit platform is reported. For individual waveguide-integrated QEs, an off-chip count rate exceeding 6 × 10 4 counts per second (cps; saturation rate >8.6 × 10 4 cps) is measured at room temperature under continuous-wave (CW) excitation. In an unpatterned thin-film sample, antibunching with g (2) (0) ∼ 0.08 and photon count rates exceeding 8 × 10 5 cps (saturation rate >1 × 10 6 cps) are measured at room temperature under CW excitation. Although spin and detailed optical line width measurements are left for future work, these results already show the potential for high-quality QEs monolithically integrated in a wide range of III-nitride device technologies that would enable new quantum device opportunities and industrial scalability.
Solid-state quantum emitters (QEs) are fundamental in photonic-based quantum information processing. There is strong interest to develop high-quality QEs in III-nitride semiconductors because of their sophisticated manufacturing driven by large and growing applications in optoelectronics, high voltage power transistors, and microwave amplifiers. Here, we report the generation and direct integration of QEs in an aluminium nitride-based photonic integrated circuit platform. For individual waveguide-integrated QEs, we measure an off-chip count rate exceeding 6×104 counts per second (cps) (saturation rate > 8.6×104 cps). In an unpatterned thin-film sample, we measure antibunching with g(2)(0)∼0.05 and photon count rates exceeding 8×105 cps (saturation rate > 1×106 cps). Although spin and detailed optical linewidth measurements are left for future work, these results already show the potential for high-quality QEs monolithically integrated in a wide range of III-nitride device technologies that would enable new quantum device opportunities and industrial scalability.
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.
Silicon is an attractive host for scalable quantum photonics, but the absence of bright telecom-band emitters with optically addressable spin states has limited its use for spin-photon interfaces. Here we demonstrate the Al1-center, an aluminum--carbon defect in silicon, as a bright waveguide-integrated single-photon emitter with a ground-state spin. Using isotopically purified silicon-on-insulator nanophotonic devices, we isolate individual Al1-centers and observe high-purity single-photon emission with g(2)(0)=0.04 without background subtraction. Time-resolved photoluminescence spectroscopy reveals a fast excited-state lifetime of 135 ns, nearly an order of magnitude shorter than the benchmark provided by the well-studied T-center. Resonant photoluminescence excitation measurements further resolve the zero-phonon transition and reveal a narrow homogeneous linewidth reaching 47 MHz, threefold narrower than the T-center under comparable temperature. Through magneto-optical spectroscopy, we resolve the spin-dependent transitions of the bound-exciton manifold and achieve spin-selective optical pumping, fulfilling the prerequisite for quantum state initialization and readout. These results establish the Al1-center as a bright telecom-band spin-photon interface in silicon photonics and introduce a promising platform for integrated quantum networks.
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.