Ultracoherent Gigahertz Diamond Spin-Mechanical Lamb Wave Resonators.

We report the development of an all-optical approach that excites the fundamental compression mode in a diamond Lamb wave resonator with an optical gradient force and detects the induced vibrations via strain coupling to a silicon vacancy center, specifically, via phonon sidebands in the optical excitation spectrum of the silicon vacancy. Sideband optical interferometry has also been used for the detection of in-plane mechanical vibrations, for which conventional optical interferometry is not effective. These experiments demonstrate a gigahertz fundamental compression mode with a Q factor of >107 at temperatures near 7 K, providing a promising platform for reaching the quantum regime of spin mechanics, especially phononic cavity quantum electrodynamics of electron spins.

Selective Generation of V2 Silicon Vacancy Centers in 4H-Silicon Carbide.

The deterministic generation of individual color centers with defined orientations or types in solid-state systems is paramount for advancements in quantum technologies. Silicon vacancies in 4H-silicon carbide (4H-SiC) can be formed in V1 and V2 types. However, silicon vacancies are typically generated randomly between V1 and V2 types with similar probabilities. Here, we show that the preferred V2 centers can be selectively generated by focused ion beam (FIB) implantation on the m-plane in 4H-SiC. When implantation is on the m-plane (a-plane), the generation probability ratio between V1 and V2 centers increase exponentially (remains constant) with decreasing FIB fluences. With a fluence of 10 ions/spot, the probability to generate V2 centers is seven times higher than V1 centers. Our results represent a critical step toward the deterministic creation of specific defect types.

Room-Temperature Photochromism of Silicon Vacancy Centers in CVD Diamond.

The silicon vacancy (SiV) center in diamond is typically found in three stable charge states, SiV0, SiV-, and SiV2-, but studying the processes leading to their formation is challenging, especially at room temperature, due to their starkly different photoluminescence rates. Here, we use confocal fluorescence microscopy to activate and probe charge interconversion between all three charge states under ambient conditions. In particular, we witness the formation of SiV0 via the two-step capture of diffusing, photogenerated holes, a process we expose both through direct SiV0 fluorescence measurements at low temperatures and confocal microscopy observations in the presence of externally applied electric fields. In addition, we show that continuous red illumination induces the converse process, first transforming SiV0 into SiV- and then into SiV2-. Our results shed light on the charge dynamics of SiV and promise opportunities for nanoscale sensing and quantum information processing.

Spontaneous Light Emission Assisted by Mie Resonances in Diamond Nanoparticles.

Spontaneous light emission is known to be affected by the local density of states and enhanced when coupled to a resonant cavity. Here, we report on an experimental study of silicon-vacancy (SiV) color center fluorescence and spontaneous Raman scattering from subwavelength diamond particles supporting low-order Mie resonances in the visible range. For the first time to our knowledge, we have measured the size dependences of the SiV fluorescence emission rate and the Raman scattering intensity from individual diamond particles in the range from 200 to 450 nm. The obtained dependences reveal a sequence of peaks, which we explicitly associate with specific multipole resonances. The results are in agreement with our theoretical analysis and highlight the potential of intrinsic optical resonances for developing nanodiamond-based lasers and single-photon sources.

Probing Charge Dynamics in Diamond with an Individual Color Center.

Control over the charge states of color centers in solids is necessary to fully utilize them in quantum technologies. However, the microscopic charge dynamics of deep defects in wide-band-gap semiconductors are complex, and much remains unknown. We utilize a single-shot charge-state readout of an individual nitrogen-vacancy (NV) center to probe the charge dynamics of the surrounding defects in diamond. We show that the NV center charge state can be converted through the capture of holes produced by optical illumination of defects many micrometers away. With this method, we study the optical charge conversion of silicon-vacancy (SiV) centers and provide evidence that the dark state of the SiV center under optical illumination is SiV2-. These measurements illustrate that charge carrier generation, transport, and capture are important considerations in the design and implementation of quantum devices with color centers and provide a novel way to probe and control charge dynamics in diamond.

Photo-Induced Charge State Dynamics of the Neutral and Negatively Charged Silicon Vacancy Centers in Room-Temperature Diamond.

The silicon vacancy (SiV) center in diamond is drawing much attention due to its optical and spin properties, attractive for quantum information processing and sensing. Comparatively little is known, however, about the dynamics governing SiV charge state interconversion mainly due to challenges associated with generating, stabilizing, and characterizing all possible charge states, particularly at room temperature. Here, multi-color confocal microscopy and density functional theory are used to examine photo-induced SiV recombination - from neutral, to single-, to double-negatively charged - over a broad spectral window in chemical-vapor-deposition (CVD) diamond under ambient conditions. For the SiV0 to SiV- transition, a linear growth of the photo-recombination rate with laser power at all observed wavelengths is found, a hallmark of single photon dynamics. Laser excitation of SiV‒, on the other hand, yields only fractional recombination into SiV2‒, a finding that is interpreted in terms of a photo-activated electron tunneling process from proximal nitrogen atoms.

Giant Quantum Electrodynamic Effects on Single SiV Color Centers in Nanosized Diamonds.

Understanding and mastering quantum electrodynamics phenomena is essential to the development of quantum nanophotonics applications. While tailoring of the local vacuum field has been widely used to tune the luminescence rate and directionality of a quantum emitter, its impact on their transition energies is barely investigated and exploited. Fluorescent defects in nanosized diamonds constitute an attractive nanophotonic platform to investigate the Lamb shift of an emitter embedded in a dielectric nanostructure with high refractive index. Using spectral and time-resolved optical spectroscopy of single SiV defects, we unveil blue shifts (up to 80 meV) of their emission lines, which are interpreted from model calculations as giant Lamb shifts. Moreover, evidence for a positive correlation between their fluorescence decay rates and emission line widths is observed, as a signature of modifications not only of the photonic local density of states but also of the phononic one, as the nanodiamond size is decreased. Correlative light-electron microscopy of single SiVs and their host nanodiamonds further supports these findings. These results make nanodiamond-SiVs promising as optically driven spin qubits and quantum light sources tunable through nanoscale tailoring of vacuum-field fluctuations.