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 together with seven equally-separated phonon replicas. Furthermore, we present first-principles calculations of the photoluminescence lineshape, which are in excellent agreement with our experimental data. To boost up the calculation accuracy and decrease the computation time, we extract the force constants using machine learning algorithms. This allows us to identify dominant modes in the lattice vibrations coupled to an excited electron during optical emission in the Si vacancy. The resonance phonon energy of 36 meV and the Debye-Waller factor of about 6% are obtained. We establish experimentally that the activation energy of the optically-induced spin polarization is given by the local vibrational energy. Our findings give insight into the coupling of electronic states to vibrational modes in SiC spin qubits, which is essential to predict their spin, optical, mechanical and thermal properties. The approach described can be applied to a large variety of spin defects with spectrally overlapped contributions in SiC as well as in other 3D and 2D materials.
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 t…
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…
Two dimensional electronic spectroscopy and transient grating measurements were performed, for the first time, on nitrogen-vacancy centers in diamond. These measurements reveal energy transfer and vibrational pathways with consequences for spin coherence.
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…
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…
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…
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 …
We present a theoretical study of vibrational and vibronic properties of a point defect in the dilute limit by means of first-principles density functional theory calculations. As an exemplar we choose the negatively charged nitrogen-vacancy center, a solid-state system that has served as a testbed for many protocols of quantum technology. We achieve low effective concentrations of defects by constructing dynamical matrices of large supercells containing tens of thousands of atoms. The main goal of the paper is to calculate luminescence and absorption lineshapes due to coupling to vibrational …
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…
Silicon-vacancy (SiV) center in diamond is a photoluminescence (PL) center with a characteristic zero-phonon line energy at 1.681 eV that acts as a solid-state single photon source and, potentially, as a quantum bit. The majority of the luminescence intensity appears in the zero-phonon line; nevertheless, about 30\% of the intensity manifests in the phonon sideband. Since phonons play an essential role in the operation of this system, it is of importance to understand the vibrational properties of the SiV center in detail. To this end, we carry out density functional theory calculations of dil…
We show that nitrogen-vacancy (NV) centers in diamond interfaced with a suspended carbon nanotube carrying a dc current can facilitate a spin-nanomechanical hybrid device. We demonstrate that strong magnetomechanical interactions between a single NV spin and the vibrational mode of the suspended nanotube can be engineered and dynamically tuned by external control over the system parameters. This spin-nanomechanical setup with strong, \emph{intrinsic} and \emph{tunable} magnetomechanical couplings allows for the construction of hybrid quantum devices with NV centers and carbon-based nanostructu…
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…
Coupling nitrogen vacancy centers in silicon carbide to nanophotonic resonators
University of Technology Sydney（悉尼科技大学）；ARC Centre of Excellence for Transformative Meta-Optical Systems（变革性超光学系统卓越研究中心）；The Australian National University（澳大利亚国立大学）
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…
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…
Color centers in diamond micro and nano structures are under investigation for a plethora of applications. However, obtaining high quality color centers in small structures is challenging, and little is known about how properties such as spin population lifetimes change during the transition from bulk to micro and nano structures. In this manuscript, we studied various ways to prepare diamond samples containing silicon vacancy centers and measured how population lifetimes of orbital states change in pillars as we varied their dimensions from approximately 1 $μ$m to 120 nm. We also researched t…
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…
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）
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…
The silicon-vacancy centre (SiV) in diamond has interesting vibronic features. We demonstrate that the zero phonon line position can be used to reliably identify the silicon isotope present in a single centre. This is of interest for quantum information applications since only the silicon 29 isotope has nuclear spin. In addition, we demonstrate that the 64 meV line is due to a local vibrational mode of the silicon atom. The presence of a local mode suggests a plausible origin of the isotopic shift of the zero phonon line.
Divacancy defects in silicon carbide have long-lived electronic spin states and sharp optical transitions, with properties that are similar to the nitrogen-vacancy defect in diamond. We report experiments on 4H-SiC that investigate all-optical addressing of spin states with the zero-phonon-line transitions. Our magneto-spectroscopy results identify the spin $S=1$ structure of the ground and excited state, and a role for decay via intersystem crossing. We use these results for demonstrating coherent population trapping of spin states with divacancy ensembles that have particular orientations in…
Spin defects in silicon carbide (SiC) with mature wafer-scale fabrication and micro/nano-processing technologies have recently drawn considerable attention. Although room temperature single-spin manipulation of colour centres in SiC has been demonstrated, the typically detected contrast is less than 2%, and the photon count rate is also low. Here, we present the coherent manipulation of single divacancy spins in 4H-SiC with a high readout contrast (-30%) and a high photon count rate (150 kilo counts per second) under ambient conditions, which are competitive with the nitrogen-vacancy (NV) cent…
Control of local lattice perturbations near optically-active defects in semiconductors is a key step to harnessing the potential of solid-state qubits for quantum information science and nanoscale sensing. We report the development of a stroboscopic scanning X-ray diffraction microscopy approach for real-space imaging of dynamic strain used in correlation with microscopic photoluminescence measurements. We demonstrate this technique in 4H-SiC, which hosts long-lifetime room temperature vacancy spin defects. Using nano-focused X-ray photon pulses synchronized to a surface acoustic wave launcher…
Recently, vacancy-related spin defects in silicon carbide (SiC) have been demonstrated to be potentially suitable for versatile quantum interface building and scalable quantum network construction. Significant efforts have been undertaken to identify spin systems in SiC and to extend their quantum capabilities using large-scale growth and advanced nanofabrication methods. Here we demonstrated a type of spin defect in the 4H polytype of SiC generated via hydrogen ion implantation with high-temperature post-annealing, which is different from any known defects. These spin defects can be optically…
We demonstrate that the spin of optically addressable point defects can be coherently driven with AC electric fields. Based on magnetic-dipole forbidden spin transitions, this scheme enables spatially confined spin control, the imaging of high-frequency electric fields, and the characterization of defect spin multiplicity. While we control defects in SiC, these methods apply to spin systems in many semiconductors, including the nitrogen-vacancy center in diamond. Electrically driven spin resonance offers a viable route towards scalable quantum control of electron spins in a dense array.
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, …
The recent discovery of color centers with optically addressable spin states in 3C silicon carbide (SiC) similar to the negatively charged nitrogen vacancy center in diamond has the potential to enable the integration of defect qubits into established wafer scale device architectures for quantum information and sensing applications. Here we demonstrate the design, fabrication, and characterization of photonic crystal cavities in 3C SiC films with incorporated ensembles of color centers and quality factor (Q) to mode volume ratios similar to those achieved in diamond. Simulations show that opti…
The controlled generation and manipulation of atom-like defects in solids has a wide range of applications in quantum technology. Although various defect centres have displayed promise as either quantum sensors, single photon emitters or light-matter interfaces, the search for an ideal defect with multi-functional ability remains open. In this spirit, we investigate here the optical and spin properties of the V1 defect centre, one of the silicon vacancy defects in the 4H polytype of silicon carbide (SiC). The V1 centre in 4H-SiC features two well-distinguishable sharp optical transitions and a…
Spectator-transition crosstalk in a spin-3/2 silicon-vacancy qudit in silicon carbide revealed by broadband Ramsey interferometry
Gwangju Institute of Science and Technology（光州科学技术院）；Linköping University（林雪平大学）；National Institutes for Quantum Science and Technology (QST)（国立量子科学和技术研究院）；Tohoku University（东北大学）；Korea Multi-purpose Accelerator Complex, Korea Atomic Energy Research Institute（韩国多功能加速器装置，韩国原子能研究所）
Cubic silicon carbide is an excellent platform for integration of defect qubits into established wafer scale device architectures for quantum information and sensing applications, where divacancy qubit, that is similar to the negatively charged nitrogen-vacancy (NV) center in diamond, has favorable coherence properties. We demonstrate by means of density functional theory calculations that divacancy in 3C SiC has superior spin-stress coupling parameters and stress sensitivity for nanoscale, quantum enhanced photonic, optoelectronic and optomechanical devices.
