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Silicon vacancy centers in 4H-silicon carbide (SiC) host a long-lived electronic spin and simultaneously possess spin-resolved optical transitions, making them a great candidate for implementing a spin-photon interface. These interfaces are an important building block of quantum networks, which in turn promise to enable secure communication and distributed quantum computing. To achieve this goal, the rate of coherently scattered photons collected from a single emitter needs to be maximized, which can be achieved by interfacing the emitter with an optical cavity. In this work, we integrate V2 centers inside a SiC membrane into a fiber-based Fabry-P\'erot microcavity. We find that SiC lends itself well to membrane fabrication, as evidenced by low surface roughness $\sigma_{\mathrm{RMS}}$ ~ 400 pm, high reproducibility, and consequentially a high cavity finesse F ~ 40 000. At cryogenic temperatures, we observe individual emitters coupling to cavity modes. We confirm their single-emitter character by measuring the second-order autocorrelation function and investigate the Purcell factor by measuring the optical lifetime as a function of the cavity-emitter detuning. We find a 13.3-fold enhancement of photons scattered into the zero-phonon line (ZPL), which could be further increased by using optimized mirror coatings, potentially opening the path towards deterministic spin-photon interaction.

Nanoelectrical and photonic integration of quantum optical components is crucial for scalable solid-state quantum technologies. Silicon carbide stands out as a material with mature quantum defects and a wide variety of applications in semiconductor industry. Here, we study the behaviour of single silicon vacancy (V2) colour centres in a metal-semiconductor (Au/Ti/4H-SiC) epitaxial wafer device, operating in a Schottky diode configuration. We explore the depletion of free carriers in the vicinity of the defect, as well as electrical tuning of the defect optical transition lines. By detecting single charge traps, we investigate their impact on V2 optical line width. Additionally, we investigate the charge-photon-dynamics of the V2 centre and find its dominating photon-ionisation processes characteristic rate and wavelength dependence. Finally, we probe the spin coherence properties of the V2 system in the junction and demonstrate several key protocols for quantum network applications. Our work shows the first demonstration of low temperature integration of a Schottky device with optical microstructures for quantum applications and paves the way towards fundamentally scalable and reproducible optical spin defect centres in solids.

Solid state quantum emitters are a prime candidate in distributed quantum technologies since they inherently provide a spin-photon interface. An ongoing challenge in the field, however, is the low photon extraction due to the high refractive index of typical host materials. This challenge can be overcome using photonic structures. Here, we report the integration of V2 centers in a cavity-based optical antenna. The structure consists of a silver-coated, 135 nm thin 4H-SiC membrane functioning as a planar cavity with a broadband resonance yielding a theoretical photon collection enhancement factor of 34. The planar geometry allows us to identify over 20 single V2 centers at room temperature with a mean (maximum) count rate enhancement factor of 9 (15). Moreover, we observe 10 V2 centers with a mean absorption linewidth below 80MHz at cryogenic temperatures. These results demonstrate a photon collection enhancement that is robust to the lateral emitter position.

Monoclinic $\beta$-Ga$_2$O$_3$ films grown on $c$-plane sapphire have been shown to exhibit six $(\bar{2}01)$-plane oriented domains, which are equally-spaced-by-rotation around the surface normal and equally-sized-by-volume that render the film optical response effectively uniaxial. We derive and discuss an optical model suitable for ellipsometry data analysis of such films. We model mid- and far-infrared ellipsometry data from undoped and electrically insulating films with an effective uniaxial dielectric tensor based on projections of all phonon modes within the rotation domains parallel and perpendicular to the sample normal, i.e., to the reciprocal lattice vector $\mathbf{g}_{\bar{2}01}$. Two effective response functions are described by model, and found sufficient to calculate ellipsometry data that best-match measured ellipsometry data from a representative film. We propose to render either effective dielectric functions, or inverse effective dielectric functions, each separately for electric field directions parallel and perpendicular to $\mathbf{g}_{\bar{2}01}$, by sums of Lorentz oscillators, which permit to determine either sets of transverse optical phonon mode parameters, or sets of longitudinal optical phonon mode parameters, respectively. Transverse optical modes common to both dielectric functions can be traced back to single crystal modes with $B_{\mathrm{u}}$ character, while modes with $A_{\mathrm{u}}$ character only appear within the dielectric function for polarization perpendicular to the sample surface. The thereby obtained parameter sets reveal all phonon modes anticipated from averaging over the six-fold rotation domains of single crystal $\beta$-Ga$_2$O$_3$, but with slightly shifted transverse optical, and completely different longitudinal optical phonon modes., Comment: 14 pgaes, 8 figures

Emitters in high refractive index materials like 4H-SiC suffer from reduced detection of photons because of losses caused by total internal reflection. Thus, integration into efficient nanophotonic structures which couple the emission of photons to a well defined waveguide mode can significantly enhance the photon detection efficiency. In addition, interfacing this waveguide to a classical fiber network is of similar importance to detect the photons and perform experiments. Here, we show a waveguide fiber interface in SiC. By careful measurements we determine efficiencies exceeding 93 % for the transfer of photons from SiC nanobeams to fibers. We use this interface to create a bright single photon source based on waveguide integrated V2 defects in 4H-SiC and achieve an overall photon count rate of 181 kilo-counts per second. We observe and quantify the strain induced shift of the ground state spin states and demonstrate coherent control of the electron spin with a coherence time of T2=42.5 $\rm\mu$s.

Quantum state readout is a key requirement for a successful qubit platform. In this work we demonstrate a high fidelity quantum state readout of a V2 center nuclear spin based on a repetitive readout technique. We demonstrate up to 99.5$\,\%$ readout fidelity and 99$\,\%$ for state preparation. Using this efficient readout we initialise the nuclear spin by measurement and demonstrate its Rabi and Ramsey nutation. Finally, we use the nuclear spin as a long lived memory for quantum sensing application of weakly coupled diatomic nuclear spin bath., Comment: 9 pages

Nuclear spins with hyperfine coupling to single electron spins are highly valuable quantum bits. In this work we probe and characterise the particularly rich nuclear spin environment around single silicon vacancy color-centers (V2) in 4H-SiC. By using the electron spin-3/2 qudit as a 4 level sensor, we identify several groups of $^{29}$Si and $^{13}$C nuclear spins through their hyperfine interaction. We extract the major components of their hyperfine coupling via optical detected nuclear resonance, and assign them to shell groups in the crystal via the DFT simulations. We utilise the ground state level anti-crossing of the electron spin for dynamic nuclear polarization and achieve a nuclear spin polarization of up to $98\pm6\,\%$. We show that this scheme can be used to detect the nuclear magnetic resonance signal of individual spins and demonstrate their coherent control. Our work provides a detailed set of parameters for future use of SiC as a multi-qubit memory and quantum computing platform., Comment: 9 pages, 4 figures, 1 SM

The negatively-charged silicon vacancy center ($\rm V_{Si}^-$) in silicon carbide (SiC) is an emerging color center for quantum technology covering quantum sensing, communication, and computing. Yet, limited information currently available on the internal spin-optical dynamics of these color centers prevents us achieving the optimal operation conditions and reaching the maximum performance especially when integrated within quantum photonics. Here, we establish all the relevant intrinsic spin dynamics of negatively charged $\rm V_{Si}^-$ center in 4H-SiC by an in-depth electronic fine structure modeling including intersystem-crossing and deshelving mechanisms. With carefully designed spin-dependent measurements, we obtain all previously unknown spin-selective radiative and non-radiative decay rates. To showcase the relevance of our work for integrated quantum photonics, we use the obtained rates to propose a realistic implementation of time-bin entangled multi-photon GHZ and cluster state generation. We find that up to 3-photon GHZ/cluster states are readily within reach using the existing nanophotonic cavity technology., Comment: 37 pages, 6 figures. Document includes Supplementary Information

Spin-active quantum emitters have emerged as a leading platform for quantum technologies. However, one of their major limitations is the large spread in optical emission frequencies, which typically extends over tens of GHz. Here, we investigate single V4+ vanadium centres in 4H-SiC, which feature telecom-wavelength emission and a coherent S=1/2 spin state. We perform spectroscopy on single emitters and report the observation of spin-dependent optical transitions, a key requirement for spin-photon interfaces. By engineering the isotopic composition of the SiC matrix, we reduce the inhomogeneous spectral distribution of different emitters down to 100 MHz, significantly smaller than any other single quantum emitter. Additionally, we tailor the dopant concentration to stabilise the telecom-wavelength V4+ charge state, thereby extending its lifetime by at least two orders of magnitude. These results bolster the prospects for single V emitters in SiC as material nodes in scalable telecom quantum networks., Comment: 29 pages, 20 figures, 2 tables

Shallow negatively charged silicon-vacancy centers have applications in magnetic quantum sensing and other quantum applications. Vacancy centers near the surface (within 100 nm) have different spin relaxation rates and optical spin polarization, affecting the optically detected magnetic resonance (ODMR) signal. This makes it essential to characterize these centers. Here we present the relevant spin properties of such centers. ODMR with a contrast of up to 6 %, which is better than the state of the art, allowed us to determine the zero field splitting, which is relevant for most sensing applications. We also present intensity-correlation data to verify that the signal originates from a single center and to extract transition rates between different electronic states.

Color centers in silicon carbide are emerging candidates for distributed spin-based quantum applications due to the scalability of host materials and the demonstration of integration into nanophotonic resonators. Recently, silicon vacancy centers in silicon carbide have been identified as a promising system with excellent spin and optical properties. Here, we in-depth study the spin-optical dynamics of single silicon vacancy center at hexagonal lattice sites, namely V1, in 4H-polytype silicon carbide. By utilizing resonant and above-resonant sub-lifetime pulsed excitation, we determine spin-dependent excited-state lifetimes and intersystem-crossing rates. Our approach to inferring the intersystem-crossing rates is based on all-optical pulsed initialization and readout scheme, and is applicable to spin-active color centers with similar dynamics models. In addition, the optical transition dipole strength and the quantum efficiency of V1 defect are evaluated based on coherent optical Rabi measurement and local-field calibration employing electric-field simulation. The measured rates well explain the results of spin-state polarization dynamics, and we further discuss the altered photoemission dynamics in resonant enhancement structures such as radiative lifetime shortening and Purcell enhancement. By providing a thorough description of V1 center's spin-optical dynamics, our work provides deep understanding of the system which guides implementations of scalable quantum applications based on silicon vacancy centers in silicon carbide., Comment: 32 pages, 12 figures

Color-center defects in silicon carbide promise opto-electronic quantum applications in several fields, such as computing, sensing and communication. In order to scale down and combine these functionalities with the existing silicon device platforms, it is crucial to consider SiC integrated optics. In recent years many examples of SiC photonic platforms have been shown, like photonic crystal cavities, film-on-insulator waveguides and micro-ring resonators. However, all these examples rely on separating thin films of SiC from substrate wafers. This introduces significant surface roughness, strain and defects in the material, which greatly affects the homogeneity of the optical properties of color centers. Here we present and test a method for fabricating monolithic single-crystal integrated-photonic devices in SiC: tuning optical properties via charge carrier concentration. We fabricated monolithic SiC n-i-n and p-i-n junctions where the intrinsic layer acts as waveguide core, and demonstrate the waveguide functionality for these samples. The propagation losses are below 14 dB/cm. These waveguide types allow for addressing color-centers over a broad wavelength range with low strain-induced inhomogeneity of the optical-transition frequencies. Furthermore, we expect that our findings open the road to fabricating waveguides and devices based on p-i-n junctions, which will allow for integrated electrostatic and radio frequency (RF) control together with high-intensity optical control of defects in silicon carbide., Comment: This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. This article appeared in Journal of Applied Physics 131, 025703 (2022) and may be found at https://aip.scitation.org/doi/10.1063/5.0077164

An outstanding challenge for color center-based quantum information processing technologies is the integration of optically-coherent emitters into scalable thin-film photonics. Here, we report on the integration of near-transform-limited silicon vacancy (V$_{\text{Si}}$) defects into microdisk resonators fabricated in a CMOS-compatible 4H-Silicon Carbide-on-Insulator platform. We demonstrate a single-emitter cooperativity of up to 0.8 as well as optical superradiance from a pair of color centers coupled to the same cavity mode. We investigate the effect of multimode interference on the photon scattering dynamics from this multi-emitter cavity quantum electrodynamics system. These results are crucial for the development of quantum networks in silicon carbide and bridge the classical-quantum photonics gap by uniting optically-coherent spin defects with wafer-scalable, state-of-the-art photonics., Comment: 8 pages, 5 figures + supplementary information

An outstanding hurdle for defect spin qubits in silicon carbide (SiC) is single-shot readout - a deterministic measurement of the quantum state. Here, we demonstrate single-shot readout of single defects in SiC via spin-to-charge conversion, whereby the defect's spin state is mapped onto a long-lived charge state. With this technique, we achieve over 80% readout fidelity without pre- or post-selection, resulting in a high signal-to-noise ratio (SNR) that enables us to measure long spin coherence times. Combined with pulsed dynamical decoupling sequences in an isotopically purified host material, we report single spin T2 > 5s, over two orders of magnitude greater than previously reported in this system. The mapping of these coherent spin states onto single charges unlocks both single-shot readout for scalable quantum nodes and opportunities for electrical readout via integration with semiconductor devices., Comment: 18 pages, 5 figures

Optically addressable spin defects in silicon carbide (SiC) are an emerging platform for quantum information processing. Lending themselves to modern semiconductor nanofabrication, they promise scalable high-efficiency spin-photon interfaces. We demonstrate here nanoscale fabrication of silicon vacancy centres (VSi) in 4H-SiC without deterioration of their intrinsic spin-optical properties. In particular, we show nearly transform limited photon emission and record spin coherence times for single defects generated via ion implantation and in triangular cross section waveguides. For the latter, we show further controlled operations on nearby nuclear spin qubits, which is crucial for fault-tolerant quantum information distribution based on cavity quantum electrodynamics., Comment: 18 pages, 4 figures

Optically active solid-state spin registers have demonstrated their unique potential in quantum computing, communication and sensing. Realizing scalability and increasing application complexity requires entangling multiple individual systems, e.g. via photon interference in an optical network. However, most solid-state emitters show relatively broad spectral distributions, which hinders optical interference experiments. Here, we demonstrate that silicon vacancy centres in semiconductor silicon carbide (SiC) provide a remarkably small natural distribution of their optical absorption/emission lines despite an elevated defect concentration of $\approx 0.43\,\rm \mu m^{-3}$. In particular, without any external tuning mechanism, we show that only 13 defects have to be investigated until at least two optical lines overlap within the lifetime-limited linewidth. Moreover, we identify emitters with overlapping emission profiles within diffraction limited excitation spots, for which we introduce simplified schemes for generation of computationally-relevant Greenberger-Horne-Zeilinger (GHZ) and cluster states. Our results underline the potential of the CMOS-compatible SiC platform toward realizing networked quantum technology applications., Comment: 7 pages, 4 figures

Nuclear spins in the solid state are both a cause of decoherence and a valuable resource for spin qubits. In this work, we demonstrate control of isolated 29Si nuclear spins in silicon carbide (SiC) to create an entangled state between an optically active divacancy spin and a strongly coupled nuclear register. We then show how isotopic engineering of SiC unlocks control of single weakly coupled nuclear spins and present an ab initio method to predict the optimal isotopic fraction which maximizes the number of usable nuclear memories. We bolster these results by reporting high-fidelity electron spin control (F=99.984(1)%), alongside extended coherence times (T2=2.3 ms, T2DD>14.5 ms), and a >40 fold increase in dephasing time (T2*) from isotopic purification. Overall, this work underlines the importance of controlling the nuclear environment in solid-state systems and provides milestone demonstrations that link single photon emitters with nuclear memories in an industrially scalable material., Comment: 25 pages, 5 figures

Silicon-vacancy qubits in silicon carbide (SiC) are emerging tools in quantum technology applications due to their excellent optical and spin properties. In this paper, we explore the effect of temperature and strain on these properties by focusing on the two silicon-vacancy qubits, V1 and V2, in 4H SiC. We apply density functional theory beyond the Born-Oppenheimer approximation to describe the temperature dependent mixing of electronic excited states assisted by phonons. We obtain polaronic gap around 5 and 22~meV for V1 and V2 centers, respectively, that results in significant difference in the temperature dependent dephasing and zero-field splitting of the excited states, which explains recent experimental findings. We also compute how crystal deformations affect the zero-phonon-line of these emitters. Our predictions are important ingredients in any quantum applications of these qubits sensitive to these effects., Comment: 8 pages, 5 figures

Quantum systems combining indistinguishable photon generation and spin-based quantum information processing are essential for remote quantum applications and networking. However, identification of suitable systems in scalable platforms remains a challenge. Here, we investigate the silicon vacancy centre in silicon carbide and demonstrate controlled emission of indistinguishable and distinguishable photons via coherent spin manipulation. Using strong off-resonant excitation and collecting photons from the ultra-stable zero-phonon line optical transitions, we show a two-photon interference contrast close to 90% in Hong-Ou-Mandel type experiments. Further, we exploit the system's intimate spin-photon relation to spin-control the colour and indistinguishability of consecutively emitted photons. Our results provide a deep insight into the system's spin-phonon-photon physics and underline the potential of the industrially compatible silicon carbide platform for measurement-based entanglement distribution and photonic cluster state generation. Additional coupling to quantum registers based on recently demonstrated coupled individual nuclear spins would further allow for high-level network-relevant quantum information processing, such as error correction and entanglement purification., Comment: Manuscript and Methods: 21 pages, 4 figures Supplementary Information: 18 pages, 6 figures, 1 table