Silicon vacancies in silicon carbide have been proposed as an alternative to nitrogen vacancy centers in diamonds for spintronics and quantum technologies. An important precondition for these applications is the initialization of the qubits into a specific quantum state. In this work, we study the optical alignment of the spin 3/2 negatively charged silicon vacancy in 6H-SiC. Using a time-resolved optically detected magnetic resonance technique, we coherently control the silicon vacancy spin ensemble and measure Rabi frequencies and spin-lattice relaxation time of all three transitions. Then to study the optical initialization process of the silicon vacancy spin ensemble, the vacancy spin ensemble is prepared in different ground states and optically excited. We describe a simple rate equation model that can explain the observed behaviour and determine the relevant rate constants.
Silicon carbide (SiC) hosts many interesting defects that can potentially serve as qubits for a range of advanced quantum technologies. Some of them have very interesting properties, making them potentially useful, e.g. as interfaces between stationary and flying qubits. Here we present a detailed overview of the relevant properties of the spins in silicon vacancies of the 6H-SiC polytype. This includes the temperature-dependent photoluminescence, optically detected magnetic resonance, and the relaxation times of the longitudinal and transverse components of the spins, during free precession a…
Silicon vacancies in silicon carbide (SiC) have been proposed as interesting candidates for quantum technology applications such as quantum sensing and quantum repeaters. SiC exists in many polytypes with different plane stacking sequences, and in each polytype, the vacancies can occupy a variety of different lattice sites. In this work, we characterize and identify the three most important charged silicon vacancies in the 6H-SiC polytype. We record the photoluminescence and continuous-wave optically detected magnetic resonance spectra at different radio-frequency power levels and different te…
Silicon carbide (SiC) has become a key player in realization of scalable quantum technologies due to its ability to host optically addressable spin qubits and wafer-size samples. Here, we have demonstrated optically detected magnetic resonance (ODMR) with resonant excitation, and clearly identified the ground state energy levels of the NV centers in 4H-SiC. Coherent manipulation of NV centers in SiC has been achieved with Rabi and Ramsey oscillations. Finally, we show the successful generation and characterization of single nitrogen vacancy (NV) center in SiC employing ion implantation. Our re…
The silicon vacancy in silicon carbide is a strong emergent candidate for applications in quantum information processing and sensing. We perform room temperature optically-detected magnetic resonance and spin echo measurements on an ensemble of vacancies and find the properties depend strongly on magnetic field. The spin echo decay time varies from less than 10 $μ$s at low fields to 80 $μ$s at 68 mT, and a strong field-dependent spin echo modulation is also observed. The modulation is attributed to the interaction with nuclear spins and is well-described by a theoretical model.
Silicon vacancy centers in silicon carbide are promising candidates for storing and manipulating quantum information. Implementation of fast quantum gates is an essential requirement for quantum information processing. In a low magnetic field, the resonance frequencies of silicon vacancy spins are in the range of a few MHz, the same order of magnitude as the Rabi frequencies of typical control fields. As a consequence, the rotating wave approximation becomes invalid and nonlinear processes like the absorption and emission of multiple photons become relevant. This work focuses on multi-photon t…
Silicon carbide is a very promising platform for quantum applications because of extraordinary spin and optical properties of point defects in this technologically-friendly material. These properties are strongly influenced by crystal vibrations, but the exact relationship between them and the behavior of spin qubits is not fully investigated. We uncover the local vibrational modes of the Si vacancy spin qubits in as-grown 4H-SiC. We apply the resonant microwave field to isolate the contribution from one particular type of defects, the so-called V2 center, and observe the zero-phonon line toge…
Single-photon emitting point defects in semiconductors have emerged as strong candidates for future quantum technology devices. In the present work, we exploit crystalline particles to investigate relevant defect localizations, emission shifting and waveguiding. Specifically, emission from 6H-SiC micro- and nanoparticles ranging from 100 nm to 5 $μ$m in size is collected using cathodoluminescence (CL), and we monitor signals attributed to the Si vacancy (V$_{\textrm{Si}}$) as a function of its location. Clear shifts in the emission wavelength are found for emitters localized in the particle ce…
The silicon monovacancy in 4H-SiC is a promising candidate for solid-state quantum information processing. We perform high-resolution optical spectroscopy on single V2 defects at cryogenic temperatures. We find favorable low temperature optical properties that are essential for optical readout and coherent control of its spin and for the development of a spin-photon interface. The common features among individual defects include two narrow, nearly lifetime-limited optical transitions that correspond to $m_s{=}\pm 3/2$ and $m_s{=}\pm 1/2$ spin states with no discernable zero-field splitting flu…
Silicon carbide (SiC)-based defects are promising for quantum communications, quantum information processing, and for the next generation of quantum sensors, as they feature long coherence times, frequencies near the telecom, and optical and microwave transitions. For such applications, the efficient initialization of the spin state is necessary. We develop a theoretical description of the spin polarization process by using the intersystem crossing of the silicon vacancy defect, which is enabled by a combination of optical driving, spin-orbit coupling, and interaction with vibrational modes. B…
The negatively charged silicon vacancy [V$_\text{Si}(-)$] in silicon carbide (SiC) is a paramagnetic and optically active defect in hexagonal SiC. V$_\text{Si}(-)$ defect possesses $S = 3/2$ spin with long spin coherence time and can be optically manipulated even at room temperature. Recently, electron spin resonance signals have been observed besides the signals associated with the V$_\text{Si}(-)$ defects in the 4H polytype of SiC. The corresponding centers share akin properties to those of the V$_\text{Si}(-)$ defects and thus they may be promising candidates for quantum technology applicat…
Hyperfine spectroscopy and fast, all-optical arbitrary state initialization and readout of a single, ten-level ${}^{73}$Ge vacancy nuclear spin qudit in diamond
The charge degree of freedom in solid-state defects fundamentally underpins the electronic spin degree of freedom, a workhorse of quantum technologies. Here we study charge state properties of individual near-surface nitrogen-vacancy (NV) centers in diamond, where NV$^{-}$ hosts the metrologically relevant electron spin. We find that NV$^{-}$ initialization fidelity varies between individual centers and over time, and we alleviate the deleterious effects of reduced NV$^{-}$ initialization fidelity via logic-based initialization. We also find that NV$^{-}$ can ionize in the dark, which compromi…
In this work, we demonstrate initialization and readout of nuclear spins via a negatively charged silicon-vacancy (SiV) electron spin qubit. Under Hartmann-Hahn conditions the electron spin polarization is coherently transferred to the nuclear spin. The readout of the nuclear polarization is observed via the fluorescence of the SiV. We also show that the coherence time of the nuclear spin (6 ms) is limited by the electron spin-lattice relaxation due to the hyperfine coupling to the electron spin. This work paves the way towards realization of building blocks of quantum hardware with an efficie…
A common impediment to qubit performance is imperfect state initialization. In the case of the diamond nitrogen-vacancy (NV) center, the initialization fidelity is limited by fluctuations in the defect's charge state during optical pumping. Here, we use real-time control to deterministically initialize the NV center's charge state at room temperature. We demonstrate a maximum charge initialization fidelity of 99.4$\pm$0.1% and present a quantitative model of the initialization process that allows for systems-level optimization of the spin-readout signal-to-noise ratio. Even accounting for the …
Ongoing efforts in quantum engineering have recently focused on integrating magnonics into hybrid quantum architectures for novel functionalities. While hybrid magnon-quantum spin systems have been demonstrated with nitrogen-vacancy (NV) centers in diamond, they have remained elusive on the technologically promising silicon carbide (SiC) platform mainly due to difficulties in finding a resonance overlap between the magnonic system and the spin centers. Here we circumvent this challenge by harnessing nonlinear magnon scattering processes in a magnetic vortex to access magnon modes that overlap …
The silicon-vacancy ($\mathrm{SiV}^-$) color center in diamond has attracted attention due to its unique optical properties. It exhibits spectral stability and indistinguishability that facilitate efficient generation of photons capable of demonstrating quantum interference. Here we show high fidelity optical initialization and readout of electronic spin in a single $\mathrm{SiV}^-$ center with a spin relaxation time of $T_1=2.4\pm0.2$ ms. Coherent population trapping (CPT) is used to demonstrate coherent preparation of dark superposition states with a spin coherence time of $T_2^\star=35\pm3$…
A theoretical approach is proposed to treat the spin dynamics in defect color centers. The method explicitly takes into account the spin dynamics in the ground state and excited state of the defect center as well as spin state dependent transitions involving the ground state and excited state, as well as an additional intermediate state. The proposed theory is applied to treat spin-dependent phenomena is silicon carbide, namely, in spin-3/2 silicon-vacancy centers, VSi or V2 centers. Theoretical predictions of magnetic field dependent photoluminescence intensity and optically detected magnetic…
We demonstrate optical spin polarization of the neutrally-charged silicon-vacancy defect in diamond ($\mathrm{SiV^{0}}$), an $S=1$ defect which emits with a zero-phonon line at 946 nm. The spin polarization is found to be most efficient under resonant excitation, but non-zero at below-resonant energies. We measure an ensemble spin coherence time $T_2>100~\mathrm{μs}$ at low-temperature, and a spin relaxation limit of $T_1>25~\mathrm{s}$. Optical spin state initialization around 946 nm allows independent initialization of $\mathrm{SiV^{0}}$ and $\mathrm{NV^{-}}$ within the same optically-addres…
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…
In this paper, we study the photoinduced switching of the nitrogen-vacancy (NV) center between two different charge states - negative (NV-) and neutral (NV0) at liquid helium temperature. The conversion of NV- to NV0 on a single defect is experimentally proven and its rate scales quadratically with power under resonant excitation. In addition, we found that resonant excitation of the neutral NV changes the charge state, recovering its negative configuration. This type of conversion significantly improves spectral stability of NV- defect and allows high fidelity initialization of the spin qubit…
Quantum technology relies on proper hardware, enabling coherent quantum state control as well as efficient quantum state readout. In this regard, wide-bandgap semiconductors are an emerging material platform with scalable wafer fabrication methods, hosting several promising spin-active point defects. Conventional readout protocols for such defect spins rely on fluorescence detection and are limited by a low photon collection efficiency. Here, we demonstrate a photo-electrical detection technique for electron spins of silicon vacancy ensembles in the 4H polytype of silicon carbide (SiC). Furthe…
Nitrogen vacancy (NV-) color centers in diamond are a prime candidate for use in quantum information devices, owing to their spin-1 ground state, straightforward optical initialization and readout, and long intrinsic coherence times in a room-temperature solid. While the 13C nuclear spin is often a dominant source of magnetic noise, we observe transitions between electron-nuclear hyperfine states of NV- centers in 99% 13C diamond that are robust to decoherence. At magnetic field strengths ranging from 550 - 900 G, these transitions are observable by optically detected magnetic resonance (ODMR)…
Optically controllable solid-state spin qubits are one of the basic building blocks for applied quantum technology. Efficient extraction of emitted photons and a robust spin-photon interface are crucial for the realization of quantum sensing protocols and essential for the implementation of quantum repeaters. Though silicon carbide (SiC) is a very promising material platform hosting highly-coherent silicon vacancy spin qubits, a drawback for their practical application is the unfavorable ordering of the electronic levels in the optically excited state. Here, we demonstrate that due to polytypi…
We propose a computational protocol for quantum simulations of Fermionic Hamiltonians on a quantum computer, enabling calculations which were previously not feasible with conventional encoding and ansatses of variational quantum eigensolvers (VQE). We combine a qubit-efficient encoding scheme mapping Slater determinants onto qubits with a modified qubit-coupled cluster ansatz and noise-mitigation techniques. Our strategy leads to a substantial improvement in the scaling of circuit gate counts and to a decrease in the number of required variational parameters, thus increasing the resilience to …
In this paper, we study the electron spin decoherence of single defects in silicon carbide (SiC) nuclear spin bath. We find that, although the natural abundance of $^{29}\rm{Si}$ ($p_{\rm{Si}}=4.7\%$) is about 4 times larger than that of $^{13}{\rm C}$ ($p_{\rm{C}}=1.1\%$), the electron spin coherence time of defect centers in SiC nuclear spin bath in strong magnetic field ($B>300~\rm{Gauss}$) is longer than that of nitrogen-vacancy (NV) centers in $^{13}{\rm C}$ nuclear spin bath in diamond. The reason for this counter-intuitive result is the suppression of heteronuclear-spin flip-flop proces…
Defects in silicon carbide (SiC) have emerged as a favorable platform for optically-active spin-based quantum technologies. Spin qubits exist in specific charge states of these defects, where the ability to control these states can provide enhanced spin-dependent readout and long-term charge stability of the qubits. We investigate this charge state control for two major spin qubits in 4H-SiC, the divacancy (VV) and silicon vacancy (Vsi), obtaining bidirectional optical charge conversion between the bright and dark states of these defects. We measure increased photoluminescence from VV ensemble…
We utilize nonlinear absorption to design all-optical protocols that improve both charge state initialization and spin readout for the nitrogen-vacancy (NV) center in diamond. Non-monotonic variations in the equilibrium charge state as a function of visible and near-infrared (NIR) optical power are attributed to competing multiphoton absorption processes. In certain regimes, multicolor illumination enhances the steady-state population of the NV's negative charge state above 90%. At higher NIR intensities, selective ionization of the singlet manifold facilitates a protocol for spin-to-charge co…
Color centers in silicon carbide have increasingly attracted attention in recent years owing to their excellent properties such as single photon emission, good photostability, and long spin coherence time even at room temperature. As compared to diamond which is widely used for holding Nitrogen-vacancy centers, SiC has the advantage in terms of large-scale, high-quality and low cost growth, as well as advanced fabrication technique in optoelectronics, leading to the prospects for large scale quantum engineering. In this paper, we report experimental demonstration of the generation of nanoscale…
We experimentally demonstrate high degree of polarization of 13C nuclear spins weakly interacting with nitrogen-vacancy (NV) centers in diamond. We combine coherent microwave excitation pulses with optical illumination to provide controlled relaxation and achieve a polarity-tunable, fast nuclear polarization of degree higher than 85% at room temperature for remote 13C nuclear spins exhibiting hyperfine interaction strength with NV centers of the order of 600 kHz. We show with the aid of numerical simulation that the anisotropic hyperfine tensor components naturally provide a route to control s…
Spin complexes comprising the nitrogen-vacancy (NV) center and neighboring spins are being considered as a building block for a new generation of spintronic and quantum information processing devices. Because assembling identical spin clusters is difficult, new strategies are in order to determine individual node structures with the highest precision. Here we use a pulse protocol to monitor the time evolution of the 13C ensemble in the vicinity of a NV center. We observe long-lived time correlations in the nuclear spin dynamics, limited by NV spin-lattice relaxation. We use the host 14N spin a…
The intersystem crossing (ISC) is an important process in many solid-state atomlike impurities. For example, it allows the electronic spin state of the nitrogen-vacancy (NV) center in diamond to be initialized and read out using optical fields at ambient temperatures. This capability has enabled a wide array of applications in metrology and quantum information science. Here, we develop a microscopic model of the state-selective ISC from the optical excited state manifold of the NV center. By correlating the electron-phonon interactions that mediate the ISC with those that induce population dyn…
The nuclear spin in the vicinity of a nitrogen-vacancy (NV) center possesses of long coherence time and convenient manipulation assisted by the strong hyperfine interaction with the NV center. It is suggested for the subsequent quantum information storage and processing after appropriate initialization. However, current experimental schemes are either sensitive to the inclination and magnitude of the magnetic field or require thousands of repetitions to achieve successful realization. Here, we propose polarizing a 13C nuclear spin in the vicinity of an NV center via a dark state. We demonstrat…
Here I present the theory of a new hybrid paramagnetic-ferrimagnetic SiC-YiG quantum sensor. It is designed to allow sub-nanoscale single external spin sensitivity optically detected pulsed electron electron double resonance spectroscopy, using an X band pulsed EPR spectrometer and an optical fiber. The sensor contains one single V2 negatively charged silicon vacancy color center in 4H-SiC, whose photoluminescence is waveguided by a 4H-SiC nanophotonic structure towards an optical fiber. This V2 spin probe is created by ion implantation at a depth of few nanometers below the surface, determine…
Engineering of Dual Wavelength, Polarization Selective Metalenses in Silicon Carbide
University of Technology Sydney（悉尼科技大学）；ARC Centre of Excellence for Transformative Meta-Optical Systems, University of Technology Sydney（悉尼大学变革性超光学系统卓越中心）；Australian Research Council Centre of Excellence for Transformative Meta-Optical Systems, Department of Electronic Materials Engineering, Research School of Physics, The Australian National University（澳大利亚国立大学电子材料工程系物理研究学院变革性超光学系统卓越中心）
Transition metal (TM) defects in silicon carbide (SiC) are a promising platform for applications in quantum technology. Some TM defects, e.g. vanadium, emit in one of the telecom bands, but the large ground state hyperfine manifold poses a problem for applications which require pure quantum states. We develop a driven, dissipative protocol to polarize the nuclear spin, based on a rigorous theoretical model of the defect. We further show that nuclear-spin polarization enables the use of well-known methods for initialization and long-time coherent storage of quantum states. The proposed nuclear-…
In this work, we present a method for targeted, maskless, and scalable fabrication of single silicon vacancy (VSi) defect arrays in silicon carbide (SiC) using focused ion beam. The resolution of implanted VSi defects is limited to a few tens of nanometers, defined by the diameter of the ion beam. Firstly, we studied the photoluminescence (PL) spectrum and optically detected magnetic resonance (ODMR) of the generated defect spin ensemble, confirming that the synthesized centers were in the desired defect state. Then we investigated the fluorescence properties of single VSi defects and our meas…
Electrically tunable, two-photon interference from remote silicon-vacancy centers in industrial silicon carbide
Friedrich-Alexander-Universität Erlangen-Nürnberg（埃尔朗根-纽伦堡大学）；Fraunhofer Institute of Integrated Systems and Device Technology (IISB)（弗劳恩霍夫集成系统和器件研究所）；Leibniz-Institut für Oberflächenmodifizierung e.V.（莱布尼茨表面改性研究所）；Luxembourg Institute of Science and Technology (LIST)（卢森堡科学与技术研究所）；University of Luxembourg（卢森堡大学）；University of Stuttgart（斯图加特大学）
Nitrogen-Vacancy (NV) centers in diamond have been identified over the past few years as promising systems for a variety of applications, ranging from quantum information science to magnetic sensing. This relies on the unique optical and spin properties of the negatively charged NV. Many of these applications require shallow NV centers, i.e. NVs that are close (a few nm) to the diamond surface. In recent years there has been increasing interest in understanding the dynamics of NV centers under various illumination conditions, specifically under infra-red (IR) excitation, which has been demonst…
Single photon emitters in silicon carbide (SiC) are attracting attention as quantum photonic systems. However, to achieve scalable devices it is essential to generate single photon emitters at desired locations on demand. Here we report the controlled creation of single silicon vacancy ($V_{Si}$) centres in 4H-SiC using laser writing without any post-annealing process. Due to the aberration correction in the writing apparatus and the non-annealing process, we generate single $V_{Si}$ centres with yields up to 30%, located within about 80 nm of the desired position in the transverse plane. We a…
