Spin-photon interfaces based on solid-state defects are key building blocks for scalable quantum networks and hybrid quantum platforms. Optimizing light-matter coupling in these systems requires precise knowledge of the optical transition dipole polarization, yet for many promising quantum emitters this quantity is hard to determine and therefore remains poorly characterized. Here, we develop a framework for reconstructing electric transition dipole polarization in spin-1/2 solid-state defects directly from ensemble spectroscopy. The approach combines the response of photoluminescence spectra to magnetic field, optical polarization, and strain. Applied to erbium ions in silicon, a particularly challenging system containing multiple crystallographic subsites, the framework identifies strain-induced shifts as the origin of asymmetric ensemble spectra and enables simultaneous determination of the optical dipole polarization and strain-orbital coupling tensor. The resulting model predicts how cavity-ion coupling depends on crystallographic orientation and magnetic-field direction, which we verify using single erbium ions coupled to a nanophotonic cavity. Together, these results establish a broadly applicable route for extracting microscopic properties of solid-state quantum emitters from ensemble spectroscopy and for engineering optimized spin-photon and spin-phonon interfaces.
Spin-photon interfaces based on solid-state defects are key building blocks for scalable quantum networks and hybrid quantum platforms. Optimizing light-matter coupling in these systems requires precise knowledge of the optical transition dipole polarization, yet for many promising quantum emitters this quantity is hard to determine and therefore remains poorly characterized. Here, we develop a framework for reconstructing electric transition dipole polarization in spin-1/2 solid-state defects directly from ensemble spectroscopy. The approach combines the response of photoluminescence spectra to magnetic field, optical polarization, and strain. Applied to erbium ions in silicon, a particularly challenging system containing multiple crystallographic subsites, the framework identifies strain-induced shifts as the origin of asymmetric ensemble spectra and enables simultaneous determination of the optical dipole polarization and strain-orbital coupling tensor. The resulting model predicts how cavity-ion coupling depends on crystallographic orientation and magnetic-field direction, which we verify using single erbium ions coupled to a nanophotonic cavity. Together, these results establish a broadly applicable route for extracting microscopic properties of solid-state quantum emitters from ensemble spectroscopy and for engineering optimized spin-photon and spin-phonon interfaces.
Hybrid quantum photonic systems connect classical photonics to the quantum world and promise to deliver efficient light-matter quantum interfaces while leveraging the advantages of both, the classical and the quantum, subsystems. However, combining efficient, scalable photonics and solid-state quantum systems with desirable optical and spin properties remains a formidable challenge. In particular, the access to individual spin states and coherent mapping to photons remains unsolved for hybrid systems. In this paper, we demonstrate all-optical initialization and readout of the electron spin of a negatively charged silicon-vacancy center in a nanodiamond coupled to a silicon nitride photonic crystal cavity. We characterize relevant parameters of the coupled emitter-cavity system and determine the silicon-vacancy center’s spin-relaxation and spin-decoherence rate. Our results mark a key step towards the realization of a hybrid spin-photon interface based on silicon nitride photonics and the silicon-vacancy center’s electron spin in nanodiamonds with potential use for quantum networks, quantum communication, and distributed quantum computation. Published by the American Physical Society 2024
Color centers are optically active point defects in semiconductor materials, many of them carrying a spin degree of freedom that couples coherently to emitted photons. This makes them a leading candidate for building quantum computers, networks, and sensors, but realizing that promise depends on the interface between the emitter and light. Color centers must be integrated into nanophotonic structures, such as nanopillars that collect their emission efficiently and optical cavities that couple them to a single mode. This dissertation studies the physics of quantum emitters inside such structures along two complementary threads: the direct cryogenic spectroscopy of color centers integrated into silicon carbide nanostructures, and the study of the physics of many-body cavity quantum electrodynamics (CQED) through simulation on superconducting and trapped-ion quantum hardware. The first thread concerns the nitrogen-vacancy (NV) center in 4H silicon carbide integrated into nanopillars. We show that the sub-wavelength geometry of a nanopillar reshapes the local electromagnetic environment, granting optical access to transitions that selection rules forbid in bulk material: emission from the PL3 divacancy, nearly absent in planar devices, becomes pronounced in nanopillars through a polarization transformation of the excitation field, and the orientation-dependent collection of the pillar resolves the previously ambiguous NV4′ line, establishing nanophotonic integration as a symmetry-sensitive probe of defect structure. We then take up the complementary problem of quantifying how many emitters a device contains, adapting the number-and-brightness technique from fluorescence microscopy to solid-state emitters. This calibration-free method counts dense NV ensembles in silicon carbide nanopillars, a regime beyond the reach of existing optical techniques, and extracts their areal density and formation yield. The second thread turns to many-body cavity QED, in which placing N emitters in a common cavity enhances the light-matter coupling by √N and gives rise to collective effects that are central to strong-coupling applications yet difficult to achieve in solid-state devices based on defects. We realize one such effect on a superconducting circuit, demonstrating photon blockade, the conversion of a coherent drive into a stream of single photons, in a Tavis–Cummings system of N = 1, 2, 3 transmon qubits coupled to a common resonator. To study the open-system dynamics that govern these systems, we digitally simulate the dissipative Tavis–Cummings model on both a superconducting and a trapped-ion processor. Platform-specific compilation and error mitigation yield population dynamics in close agreement with exact solutions, providing a recipe for simulating cavity-emitter systems on contemporary quantum computers. Together, the two threads connect the fabrication and characterization of color-center devices to the many-body cavity-QED physics that will ultimately govern their performance.
Summary form only given. Although it is often assumed that all light-matter interactions at optical frequencies are mediated by electric dipole transitions, strong optical-frequency magnetic dipoles do exist. In fact, we see magnetic dipole emission every day from the many lanthanide ions (such as erbium, europium, and terbium) that help to illuminate everything from fluorescent lighting to telecom fiber amplifiers. Higher-order processes such as magnetic dipole and electric quadrupole transitions also play an important part in the light emission from transition metal ions and semiconductor quantum dots. Nevertheless, most applications have overlooked the device implications of these electric-dipole-forbidden transitions throughout the visible and near-infrared regime, and their contributions to many important emitters have not been fully characterized.In this presentation, we will experimentally characterize the "forbidden" transitions in a range of solid-state emitters and investigate their applications and implications for nanophotonics. We will examine the electric dipole approximation commonly used to describe light-matter interactions and discuss naturally occurring systems that exhibit higher-order magnetic dipole and electric quadrupole emission. We will illustrate how these nanoscale quantum transitions can provide both a new way to probe magnetic light-matter interactions and a new degree of design freedom for active electronic and photonic devices. Specifically, we will demonstrate how the different symmetries of multipolar transitions can be exploited to identify, quantify, and control light emission, even at sub-lifetime scales. Despite similar radiation patterns, magnetic and electric dipole emitters have different symmetries with respect to polarization and phase. Thus, in an inhomogeneous environment, we can tailor interference effects and the local density of optical states to selectively enhance either electric or magnetic dipole emission [1,2]. To examine the scope of such higher-order transitions, we will present quantum mechanical calculations that identify all the magnetic dipole and electric quadrupole emission lines in the trivalent lanthanide series in the visible to near-infrared spectrum [3]. Then, we will present an energyand momentum-resolved spectroscopy technique to directly quantify the electric and magnetic dipole contributions from any mixed transition. [4] Using energy-momentum spectroscopy, we will experimentally examine the higher order transitions in lanthanide ions [4,5], transition metal ions [6], and epitaxial quantum dots [7]. If time permits, we will then show how the symmetry differences between magnetic and electric dipoles can be used to address specific electronic states [6] and to dynamically tune emission spectra at sub-lifetime-scales [8].
Quantum emitters in solid-state crystals have recently attracted a lot of attention due to their simple applicability in optical quantum technologies. The polarization of single photons generated by quantum emitters is one of the key parameters that play a crucial role in the applications, such as quantum computation that uses the indistinguishability of photons. However, the degree of single photon polarization is typically quantified using time-averaged photoluminescence intensity of single emitters, which provides limited information about the dipole properties in solids. In this work, we use single defects in hexagonal boron nitride and nanodiamond as efficient room-temperature single photon sources to reveal the origin and the temporal evolution of dipole orientation in solid-state quantum emitters. The angle of excitation and emission dipoles relative to the crystal axes are determined experimentally and then calculated using density functional theory, which results in characteristic angles for every specific defect that can be used as an efficient tool for defect identification and understanding their atomic structure. Moreover, the temporal polarization dynamics reveal a strongly modified linear polarization visibility that depends on the excited state decay time of individual excitation. This effect can be traced back potentially to the excitation of excess charges in the local crystal environment. Understanding such hidden time-dependent mechanisms can further be used to improve the performance of polarization-sensitive experiments, in particular that of quantum communication with single photon emitters.
Harnessing rare-earth ions in oxides for quantum networks requires integration with bright emitters in III-V semiconductors, but local disorder and interfacial noise limit their optical coherence. Here, we investigate the microscopic origins of the ensemble spectrum in Er3+:TiO2 epitaxial thin films on GaAs and GaSb substrates. Ab initio calculations combined with noise-Hamiltonian modeling and Monte Carlo simulations quantify the effects of interfacial and bulk spin noise and local strain on erbium crystal-field energies and inhomogeneous linewidths. Photoluminescence excitation spectroscopy reveals that Er3+ ions positioned at increasing distances from the III-V/oxide interface produce a systematic blue shift of the Y1→Z1 transition, consistent with strain relaxation predicted by theory. Thermal annealing produces a compensating redshift and linewidth narrowing, isolating the roles of oxygen-vacancy and gallium-diffusion noise. These results provide microscopic insight into disorder-driven decoherence, offering pathways for precise control of hybrid quantum systems for scalable quantum technologies.
The ability to control solid-state quantum emitters is fundamental to advancing quantum technologies. The performance of these systems is fundamentally governed by their spin-dependent photodynamics, yet conventional control methods using cavities offer limited access to key non-radiative processes. Here we demonstrate that anisotropic lattice strain serves as a powerful tool for manipulating spin dynamics in solid-state systems. Under high pressure, giant shear strain gradients trigger a complete reversal of the intrinsic spin polarization, redirecting ground-state population from ∣0⟩ to ∣±1⟩ manifold. We show that this reprogramming arises from strain-induced mixing of the NV center's excited states and dramatic alteration of intersystem crossing, which we quantify through a combination of opto-magnetic spectroscopy and a theoretical model that disentangles symmetry-preserving and symmetry-breaking strain contributions. Furthermore, the polarization reversal is spatially mapped with a transition region below 120 nm, illustrating sub-diffraction-limit control. Our work establishes strain engineering as a powerful tool for tailoring quantum emitter properties, opening avenues for programmable quantum light sources, high-density spin-based memory, and hybrid quantum photonic devices.