Erbium ion is among the most promising solid-state single photon emitters and spin-photon interfaces for quantum networks, emitting directly in the telecom C-band in many host semiconductors. Recently, the search for scalable, low-noise host materials turned toward atomically thin and van der Waals materials that enable efficient integration with nanophotonic architectures. Here, we identify talc, a naturally occurring layered magnesium silicate, as a promising host for telecom-active erbium centers. Using first-principles density functional theory combined with multireference wavefunction calculations, we investigate the thermodynamic stability, electronic structure, crystal-field splitting, and optical transitions of erbium-related defects in talc. We find that substitutional incorporation of Er at Mg sites is energetically favourable over a wide range of Fermi-levels, leading predominantly to telecom C band emitting Er^3+ configuration. The characteristic ^4I_13/2→^4I_15/2 transition of Er^3+ is preserved in the talc environment and remains centred near 1.55 μm, while crystal-field interactions produce a Stark manifold suitable for spectrally selective optical addressing. The combination of thermodynamic stability, wide band gap, low background emission, and compatibility with van der Waals heterostructures suggests that erbium-doped talc constitutes a promising platform for integrated photonics in the C-band.

Color centers in wide-bandgap semiconductors are promising spin-photon interfaces for quantum repeater nodes, but their optical coherence is highly sensitive to the local cryogenic environment. We characterize the thermal performance of a closed-cycle microscope cryostat with an in-vacuum room-temperature objective using the V1 center in 4H-SiC. Using pulsed resonant photoluminescence excitation of single V1 centers, we extract the zero-phonon-line linewidth as a local probe of the effective sample temperature. Comparing linewidths for different mounting media and objective geometries at a fixed cold-stage thermometer reading below 6 K, we find that both the thermal interface and the objective working distance strongly affect the thermal margin at the emitter. Linewidths vary by more than an order of magnitude between configurations, consistent with several-kelvin differences within a phonon-activated linewidth model. These results provide a simple spectroscopic diagnostic and practical guidelines for configuring cryogenic optical platforms for solid-state quantum networks.

Color center spins in 4H-SiC offer a rare combination of wafer-scale materials maturity with long spin coherence and chip-level photonics, making them promising building blocks for scalable quantum technologies. In particular, the silicon vacancy hosts an S=3/2 ground state, a native qudit that enables compact encodings and subspace-selective control, but also introduces spectator transitions: short, detuned pulses can coherently drive non-addressed level pairs and create crosstalk. Here we use broadband Ramsey interferometry to reveal and quantify such spectator-transition crosstalk. Experimentally, the Ramsey Fourier spectra display multiple lines beyond the addressed single-quantum transition. Analytically, we map each line to a pairwise energy difference between qudit levels of the rotating-frame Hamiltonian and assign its weight via compact amplitudes set by the prepared state and the microwave pulse parameters, predicting a deterministic six-branch structure. Numerical time-domain propagation with the experimental sampling reproduces the detuning map, and the measured peak positions coincide with the analytic branch lines without frequency fitting. Together these results provide a practical, spectator-aware framework for multilevel control in the silicon vacancy qudit. The approach offers clear guidance to suppress crosstalk or, conversely, to exploit spectator lines, for example as additional constraints for in situ pulse calibration and for phase-sensitive quantum state and process estimation.

Point defects in silicon carbide (SiC), particularly the negatively-charged silicon vacancy () in 4H-SiC, are leading candidates for scalable quantum technologies due to their favorable spin-optical properties and compatibility with industrial semiconductor fabrication processes. Comprehensive knowledge of a defect's electronic structure is essential for interpreting spin-optical dynamics and for the reliable design and optimization of defect-based quantum devices. Despite extensive study, our knowledge of the electronic structure of is limited since key excited-state manifolds have remained inaccessible to conventional steady-state spectroscopy. In this study, transient absorption spectroscopy is utilized to probe non-equilibrium electronic transitions of and to uncover previously unobserved excited states. The first direct observation of the elusive quartet transition is presented, with its broad spectral signature attributed to nonadiabatic vibronic coupling. Within the spin-doublet manifold, which is central to optically detected magnetic resonance (ODMR) but has remained unresolved spectroscopically, multiple optical transitions are identified. The complete electronic level structure in the relevant energy range is elucidated by combining polarization-resolved spectroscopy, group-theoretical analysis, quantum embedding calculations, and first-principles optical lineshape modeling. Collectively, these results provide a microscopic understanding of the electronic structure. Our approach also establishes a general framework for resolving and understanding complex excited-state manifolds in wide-bandgap color centers.

The divacancies in 4H-SiC attract significant attention for use as qubits owing to their spin and photoluminescence (PL) properties and near telecom PL emission. Nevertheless, there exist some ambiguities in the interpretation of their optically detected magnetic resonance (ODMR) spectra, especially at elevated temperatures. In this study, we investigate the divacancy configurations PL1-PL7 using PL and ODMR. We record the full temperature dependence between liquid-helium temperature (3.8 K) and room temperature (295 K), obtained with two different laser energies and different laser polarizations. We also present PL data recorded simultaneously with the ODMR. Our study allows us to continuously follow the evolution of all divacancy configurations in ODMR with temperature, even though their signature is not distinguishable in PL at elevated temperatures. We identify all lines in the room-temperature ODMR spectrum and show that a hypothetical defect PL7, assumed in earlier work to stem from another divacancy configuration, does not exist and its ODMR signal at room temperature is fully explained with PL4. We also provide direct PL evidence on the spatial distribution of PL5, PL6, and a new PL3a defect, showing their presence only close to the surface of the sample, thus corroborating their association with divacancies near stacking faults. We address also the role of the upconversion of the photoluminescence in the ODMR spectra observed at higher temperatures.

The spectral characterization of quantum emitter luminescence over broad wavelength ranges and fast timescales is important for applications ranging from biophysics to quantum technologies. Here we present the application of time-domain Fourier transform spectroscopy, based on a compact and stable birefringent interferometer coupled to low-dark-count superconducting single-photon detectors, to the study of quantum emitters. We experimentally demonstrate that the system enables spectroscopy of quantum emitters over a broad wavelength interval from the near-infrared to the telecom range, where grating-based spectrometers coupled to InGaAs cameras are typically noisy and inefficient. We further show that the high temporal resolution of single-photon detectors, which can be on the order of tens of picoseconds, enables the monitoring of spin-dependent spectral changes on sub-nanosecond timescales.

The divacancy comprising two neighboring vacant sites in the SiC lattice is a promising defect for applications in quantum technology. So far, most work is concerned with the divacancy in 4H-SiC, whereas the divacancies in 6H- and 3C-SiC have received much less attention. Here, we outline arguments showing that the neutral charge state of the divacancies in the latter two polytypes is intrinsically stable, in contrast to that in 4H-SiC where the photoluminescence quenches in most materials for certain excitation energies (below approximately 1.3 eV). Divacancies in 6H- and 3C-SiC are anticipated to remain stable even with resonant excitation. We provide new ab initio calculation results for the charge transfer levels of divacancies in 6H- and 3C-SiC. Using the temperature dependence of the divacancy emission in 3C-SiC, we estimate the energy position of the (+|0) charge transfer level of the divacancy within the bandgap of this polytype and compare with theoretical results.

Quantum communication promises unprecedented communication capabilities enabled by the transmission of quantum states of light. However, current implementations face severe limitations in communication distance due to photon loss. Silicon carbide (SiC) defects have emerged as a promising quantum device platform, offering strong optical transitions, long spin coherence lifetimes and the opportunity for integration with semiconductor devices. Some defects with optical transitions in the telecom range have been identified, allowing to interface with fiber networks without the need for wavelength conversion. These unique properties make SiC an attractive platform for the implementation of quantum nodes for quantum communication networks. We provide an overview of the most prominent defects in SiC and their implementation in spin-photon interfaces. Furthermore, we model a memory-enhanced quantum communication protocol in order to extract the parameters required to surpass a direct point-to-point link performance. Based on these insights, we summarize the key steps required towards the deployment of SiC devices in large-scale quantum communication networks.

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 initialize 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 a weakly coupled diatomic nuclear-spin bath.

Vanadium in silicon carbide (SiC) is emerging as an important candidate system for quantum technology due to its optical transitions in the telecom wavelength range. However, several key characteristics of this defect family including their spin relaxation lifetime (T1), charge state dynamics, and level structure are not fully understood. In this work, we determine the T1 of an ensemble of vanadium defects, demonstrating that it can be greatly enhanced at low temperature. We observe a large spin contrast exceeding 90% and long spin-relaxation times of up to 25s at 100mK, and of order 1s at 1.3K. These measurements are complemented by a characterization of the ensemble charge state dynamics. The stable electron spin furthermore enables high-resolution characterization of the systems' hyperfine level structure via two-photon magneto-spectroscopy. The acquired insights point towards high-performance spin-photon interfaces based on vanadium in SiC.

Nuclear spins with hyperfine coupling to single electron spins are highly valuable quantum bits. Here we probe and characterize 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 four level sensor, we identify several sets 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 magnetic resonance, and assign them to shells in the crystal via the density function theory simulations. We utilize the ground-state level anticrossing of the electron spin for dynamic nuclear polarization and achieve a nuclear-spin polarization of up to 98±6%. 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 and first steps for future use of SiC as a multiqubit memory and quantum computing platform.

In this study, we address selection rules with respect to the polarization of the optical excitation of two color centers in 4H−SiC and 6H−SiC with potential for applications in quantum technology, the divacancy and the nitrogen-vacancy pair. We show that the photoluminescence of the axial configurations of higher symmetry (C3v) than the basal ones (C1h) can be canceled using any excitation (resonant or nonresonant) with polarization parallel to the crystal axis (EL||c). The polarization selection rules are determined using group-theoretical analysis and simple physical arguments showing that phonon-assisted absorption with EL||c is prohibited despite being formally allowed by group theory. A comparison with the selection rules for the silicon vacancy, another defect with C3v symmetry, is also carried out. Using the selection rules, we demonstrate selective excitation of only one basal divacancy configuration in 4H−SiC, the PL3 line, and discuss the higher contrast and increased Debye-Waller factor in the selectively excited spectrum. Published by the American Physical Society 2024

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.

Silicon carbide (SiC) has long been developed for applications in power devices and is the only wide-bandgap semiconductor with commercially available substrates of all types, high-purity semi-insulating, n- and p-type conductive. Since the last decade, SiC has emerged also as a promising material platform for applications in quantum technology, such as quantum sensing and quantum communication, for it hosts various optical centers with favorable optical and spin properties for spin quantum bits that have long spin coherence times and can be controlled optically or electrically. This has led to more intensive optical and electrical characterization, and characterization using magnetic techniques on several point defects in recent years with new data frequently reported. In this scope, we give an overview on photoluminescent centers that emit light near and at telecom wavelengths, provide updated information on their identification, and discuss the underlying defect physics with a focus on the electronic structure and optical properties. The overviewed defects include two intrinsic defects (the silicon vacancy and the divacancy), several transition metals in SiC (V, Cr, Mo, W, Nb) and the rare-earth Er, as well as the nitrogen-vacancy pair in SiC, with insight to their possible application in quantum communication. Some unidentified defects with near-infrared emission are also briefly reviewed.

Paramagnetic defects and nuclear spins are often the major sources of decoherence and spin relaxation in solid-state qubits realized by optically addressable point defect spins in semiconductors. It is commonly accepted that a high degree of depletion of nuclear spins can enhance the coherence time by reducing magnetic noise. Here we show that the isotope purification beyond a certain optimal level becomes contra-productive, when both electron and nuclear spins are present in the vicinity of the qubits. Using state-of-the-art numerical tools and considering the silicon vacancy qubit in various spin environments, we demonstrate that the coupling to spin-1/2 point defects in the lattice can be significantly enhanced by isotope purification. The enhanced coupling shortens the spin relaxation time that in turn may limit the the coherence time of spin qubits. Our results can be straightforwardly generalized to triplet point defect qubits, such as the NV center in diamond and the divacancy in SiC.

In this study, we address the selection rules with respect to the polarization of the optical excitation of two colour centres in 4H-SiC and 6H-SiC with potential for applications in quantum technology, the divacancy and the nitrogen-vacancy pair. We show that the photoluminescence (PL) of the axial configurations of higher symmetry (C3v) than the basal ones (C1h) can be cancelled using any excitation (resonant or non-resonant) with polarization parallel to the crystal axis (EL||c). The polarization selection rules are determined using group-theoretical analysis and simple physical arguments showing that phonon-assisted absorption with EL||c is prohibited despite being formally allowed by group theory. A comparison with the selection rules for the silicon vacancy, another defect with C3v symmetry, is also carried out. Using the selection rules, we demonstrate selective excitation of only one basal divacancy configuration in 4H-SiC, the P3 line and discuss the higher contrast and increased Debye-Waller factor in the selectively excited spectrum.

We investigate the optical properties of vanadium single defects in SiC. We provide the first experimental verification of its optical selection rules and observe surprising sub-GHz photoluminescence inhomogeneous distributions, critical for telecom quantum technology applications.

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.

Paramagnetic defects and nuclear spins are the major sources of magnetic field-dependent spin relaxation in point defect quantum bits. The detection of related optical signals has led to the development of advanced relaxometry applications with high spatial resolution. The nearly degenerate quartet ground state of the silicon vacancy qubit in silicon carbide (SiC) is of special interest in this respect, as it gives rise to relaxation rate extrema at vanishing magnetic field values and emits in the first near-infra-red transmission window of biological tissues, providing an opportunity for developing novel sensing applications for medicine and biology. However, the relaxation dynamics of the silicon vacancy center in SiC have not yet been fully explored. In this paper, we present results from a comprehensive theoretical investigation of the dipolar spin relaxation of the quartet spin states in various local spin environments. We discuss the underlying physics and quantify the magnetic field and spin bath dependent relaxation time T_1. Using these findings we demonstrate that the silicon vacancy qubit in SiC can implement microwave-free low magnetic field quantum sensors of great potential.

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 postselection, resulting in a high signal-to-noise ratio 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 > 5 seconds, 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.