Vibronic states and their effect on the temperature and strain dependence of silicon-vacancy qubits in 4H silicon carbide
Péter Udvarhelyi, Gergő Thiering, Naoya Morioka, Charles Babin, Florian Kaiser, Daniil Lukin, Takeshi Ohshima, Jawad Ul-Hassan, Nguyen Tien Son, Jelena Vučković… 展开作者
Péter Udvarhelyi, Gergő Thiering, Naoya Morioka, Charles Babin, Florian Kaiser, Daniil Lukin, Takeshi Ohshima, Jawad Ul-Hassan, Nguyen Tien Son, Jelena Vučković, Jörg Wrachtrup, Adam Gali
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.
Silicon vacancy in silicon carbide has drawn much attention for various quantum sensing. However, most of the previous experiments are achieved using confocal scanning systems, which limit its applications in practical applications. In this work, we demonstrate a compact fiber-integrated silicon carbide silicon vacancy-based vector magnetometer at room temperature. First, we effectively couple the silicon vacancy in a tiny silicon carbide slice to an optical fiber tip and realize the readout of the spin signal through the fiber at the same time. We then study the optically detected magnetic re…
Silicon Carbide is a promising host material for spin defect based quantum sensors owing to its commercial availability and established techniques for electrical and optical microfabricated device integration. The negatively charged silicon vacancy is one of the leading spin defects studied in silicon carbide owing to its near telecom photoemission, high spin number, and nearly temperature independent ground state zero field splitting. We report the realization of nanoTesla shot-noise limited ensemble magnetometry based on optically detected magnetic resonance with the silicon vacancy in 4H si…
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 …
Precise generation of spin defects in solid-state systems is essential for nanostructure fluorescence enhancement. We investigated a method for creating single silicon vacancy defect arrays in silicon carbide using a helium-ion microscope. Maskless and targeted generation can be realized by precisely controlling the focused He+ ion beam with an implantation uncertainty of 60 nm. The generated silicon vacancies were identified by measuring the optically detected magnetic resonance spectrum and room temperature photoluminescence spectrum. We systematically studied the effects of the implantation…
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…
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…
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…
Defects in silicon carbide have been explored as promising spin systems in quantum technologies. However, for practical quantum metrology and quantum communication, it is critical to achieve the on-demand shallow spin-defect generation. In this work, we present the generation and characterization of shallow silicon vacancies in silicon carbide by using different implanted ions and annealing conditions. The conversion efficiency of silicon vacancy of helium ions is shown to be higher than that by carbon and hydrogen ions in a wide implanted fluence range. Furthermore, after optimizing annealing…
Solid-state color centers with manipulatable spin qubits and telecom-ranged fluorescence are ideal platforms for quantum communications and distributed quantum computations. In this work, we coherently control the nitrogen-vacancy (NV) center spins in silicon carbide at room temperature, in which telecom-wavelength emission is detected. We increase the NV concentration six-fold through optimization of implantation conditions. Hence, coherent control of NV center spins is achieved at room temperature and the coherence time T2 can be reached to around 17.1 μs. Furthermore, investigation of fluor…
Pressure-induced magnetic phase transition is attracting interest due to its ability to detect superconducting behaviour at high pressures in diamond anvil cells. However, detection of the local sample magnetic properties is a great challenge due to the small sample chamber volume. Recently, optically detected magnetic resonance (ODMR) of nitrogen vacancy (NV) centers in diamond have been used for in-situ pressure-induced phase transition detection. However, owing to their four orientation axes and temperature-dependent zero-field-splitting, interpreting the observed ODMR spectra of NV centers…
Optically interfaced spins in the solid promise scalable quantum networks. Robust and reliable optical properties have so far been restricted to systems with inversion symmetry. Here, we release this stringent constraint by demonstrating outstanding optical and spin properties of single silicon vacancy centres in silicon carbide. Despite the lack of inversion symmetry, the system's particular wave function symmetry decouples its optical properties from magnetic and electric fields, as well as from local strain. This provides a high-fidelity spin-to-photon interface with exceptionally stable an…
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 contr…
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…
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.
Silicon carbide is a promising platform for single photon sources, quantum bits (qubits) and nanoscale sensors based on individual color centers. Towards this goal, we develop a scalable array of nanopillars incorporating single silicon vacancy centers in 4H-SiC, readily available for efficient interfacing with free-space objective and lensed-fibers. A commercially obtained substrate is irradiated with 2 MeV electron beams to create vacancies. Subsequent lithographic process forms 800 nm tall nanopillars with 400-1,400 nm diameters. We obtain high collection efficiency, up to 22 kcounts/s opti…
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-de…
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.
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.
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）
We introduce an advanced material system for the production and spectroscopy of single silicon vacancy (SiV) color centers in diamond. We use microwave plasma chemical vapor deposition to synthesize heteroepitaxial nanodiamonds of approx. 160 nm in lateral size with a thickness of approx. 75 nm. These oriented 'nanoislands' combine the enhanced fluorescence extraction from subwavelength sized nanodiamonds with defined crystal orientation. The investigated SiV centers display narrow zero-phonon-lines down to 0.7 nm in the wavelength range 730-750 nm. We investigate in detail the phonon-coupling…
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…
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）
Point defects in silicon carbide are rapidly becoming a platform of great interest for single photon generation, quantum sensing, and quantum information science. Photonic crystal cavities (PCC) can serve as an efficient light-matter interface both to augment the defect emission and to aid in studying the defects' properties. In this work, we fabricate 1D nanobeam PCCs in 4H-silicon carbide with embedded silicon vacancy centers. These cavities are used to achieve Purcell enhancement of two closely spaced defect zero-phonon lines (ZPL). Enhancements of >80-fold are measured using multiple techn…
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）
We investigate phonon induced electronic dynamics in the ground and excited states of the negatively charged silicon-vacancy ($\mathrm{SiV}^-$) centre in diamond. Optical transition line widths, transition wavelength and excited state lifetimes are measured for the temperature range 4-350 K. The ground state orbital relaxation rates are measured using time-resolved fluorescence techniques. A microscopic model of the thermal broadening in the excited and ground states of the $\mathrm{SiV}^-$ centre is developed. A vibronic process involving single-phonon transitions is found to determine orbita…
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 …
Color centers in wide-bandgap semiconductors are attractive systems for quantum technologies since they can combine long-coherent electronic spin and bright optical properties. Several suitable centers have been identified, most famously the nitrogen-vacancy defect in diamond. However, integration in communication technology is hindered by the fact that their optical transitions lie outside telecom wavelength bands. Several transition-metal impurities in silicon carbide do emit at and near telecom wavelengths, but knowledge about their spin and optical properties is incomplete. We present all-…
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 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…
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…
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…
Photoluminescence (PL) spectra of single silicon vacancy (SiV) centers frequently feature very narrow room temperature PL lines in the near-infrared (NIR) spectral region, mostly between 820 nm and 840 nm, in addition to the well known zero-phonon-line (ZPL) at approx. 738 nm [E. Neu et al., Phys. Rev. B 84, 205211 (2011)]. We here exemplarily prove for a single SiV center that this NIR PL is due to an additional purely electronic transition (ZPL). For the NIR line at 822.7 nm, we find a room temperature linewidth of 1.4 nm (2.6 meV). The line saturates at similar excitation power as the ZPL. …
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 …
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 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…
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…
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…
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 present a method relying on shortcuts to adiabaticity to achieve quantum detection of high frequency signals at the nanoscale in a robust manner. More specifically, our protocol delivers tailored amplitudes and frequencies for control fields that, firstly, enable the coupling of the sensor with high-frequency signals and, secondly, minimise errors that would otherwise spoil the detection process. To exemplify the method, we particularise to detection of signals emitted by fast-rotating nuclear spins with nitrogen vacancy center quantum sensors. However, our protocol is straightforwardly app…
Progress with quantum technology has for a large part been realized with the nitrogen-vacancy centre in diamond. Part of its properties, however, are nonideal and this drives research into other spin-active crystal defects. Several of these come with much stronger energy scales for spin-orbit and hyperfine coupling, but how this affects their spin coherence is little explored. Vanadium in silicon carbide is such a system, with technological interest for its optical emission at a telecom wavelength and compatibility with semiconductor industry. Here we show coherent spin dynamics of an ensemble…
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…
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…
