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Applied Physics Letters

Coherence of NV defects in isotopically enriched 6H-28SiC at ambient conditions

Fadis F. Murzakhanov, Georgy Vladimirovich Mamin, Margarita A. Sadovnikova, E. N. Mokhov, Sergey S. Nagalyuk, Marat Revgerovich Gafurov, V. A. Soltamov

Published Nov 11, 2024• 5 citations
Publisher

Abstract

The unique spin-optical properties of NV defects in SiC, coupled with silicon carbide's advanced technology compared to diamond, make them a promising candidate for quantum technology applications. In this study, using photoinduced pulse ESR at 94 GHz (3.4 T), we reveal the room temperature spin coherence of NV defects in 6H-28SiC, purified to reduce 29Si concentration to ≈1%, four times below its natural level. We demonstrate room temperature (300 K) Hahn-echo coherence time T2 = 23.6 μs, spin–lattice relaxation time T1 = 0.1 ms, and coherent control over optically polarized NV spin states through Rabi nutation experiments. We reveal long inhomogeneous dephasing time T2* = 1.5 μs, which is about five times greater than that measured for NV defects in SiC with natural isotopic content. Our observations highlight again the potential of NV defects in 6H-28SiC, which exhibit near-infrared optical excitation and emission properties compatible with O-band fiber optics, as promising candidates for applications in quantum sensing, communication, and computation.

DOI
10.1063/5.0222098

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The unique spin-optical properties of NV defects in SiC, coupled with silicon carbide's advanced technology compared to diamond, make them a promising candidate for quantum technology applications. In this study, using photoinduced pulse ESR at 94 GHz (3.4 T), we reveal the room temperature spin coherence of NV defects in 6H-28SiC, purified to reduce 29Si concentration to ≈1%, four times below its natural level. We demonstrate room temperature (300 K) Hahn-echo coherence time T2 = 23.6 μs, spin–lattice relaxation time T1 = 0.1 ms, and coherent control over optically polarized NV spin states through Rabi nutation experiments. We reveal long inhomogeneous dephasing time T2* = 1.5 μs, which is about five times greater than that measured for NV defects in SiC with natural isotopic content. Our observations highlight again the potential of NV defects in 6H-28SiC, which exhibit near-infrared optical excitation and emission properties compatible with O-band fiber optics, as promising candidates for applications in quantum sensing, communication, and computation.
Solid-state spin defects in semiconductor matrices have become a robust medium for holding electron qubit ensembles. In this paper, the features of NV centers’ spin polarization in a silicon carbide 6 H -SiC crystal, and the laser excitation influence on the coherent properties of the color center were studied by the photoinduced pulsed EPR spectroscopy (W-band, 94 GHz). After the optical pulse, in the dark-mode regime, the characteristic time of the spin-phonon interaction of NV defects with the local environment lengthens by 1 order of magnitude compared to continuous laser irradiation, reaching a value of T 1 = 0.74 s at temperature of 50 K. An extremely efficient spin polarization (> 90%) of NV centers was discovered, which is necessary for establishing the initial pure quantum state. The obtained spin-optical and coherent properties delineate the time domain of multipulse quantum manipulations involving optical and microwave sources for promising NV centers in quantum photonics.
Among the possible defects that can occur in diamonds, one that draws attention is the nitrogen-vacancy (NV) center.Studied since the early 90s, in recent years, they became one of the most promising platforms for field applications of quantum technology at room temperature, especially for quantum sensing.They are sensitive to electric and magnetic fields, temperature, and strain, making these nanosensors a versatile platform for many applications.The NV center's spin state is easy to read and manipulate by optical means, and, most interestingly, it works well at room temperature, which facilitates its use.The great challenge to implement quantum protocols and quantum algorithms is the coherence time of the quantum states.The NV center stands out for having relatively high coherence times at room temperature.This dissertation presents measurements to characterize the electron spin coherence of NV centers in an ultrapure sample of diamond designed for quantum sensing applications.These measurements combine optical e magnetic resonance techniques.For that, a method was implemented using a conventional CCD camera and a clever imaging protocol, making it possible to perform various pulsed microwave experiments on the electron spin, such as Rabi oscillations and Hahn spin-echo, which were used for determining the characteristic relaxation times (T 1 and T 2 ).Results show that this system provides at least two readily accessible qubits that can be used in quantum protocols even at room temperature.
Defect based qubit systems like the nitrogen vacancy center in diamond have recently emerged as promising candidates for quantum technologies due to their combination of long coherence times, room temperature operation, and robust optical interface. In order to realize many of their proposed applications, defect qubits must be incorporated into scalable devices architectures consisting of photonic, mechanical, or electrical degrees of freedom. Despite much recent progress, many challenges remain for diamond growth and device fabrication. As an alternate approach, we engaged in a search for nitrogen vacancy center analogues in alternative materials with the hope of obtaining a greater degree of control over defect and material properties. Ultimately, we discovered that divacancy-related point defects in all three of the most common forms of silicon carbide- termed 4H, 6H, and 3C- act as analogues to the nitrogen vacancy center in diamond. We chose to focus our research primarily on defects in 3C silicon carbide (termed 'Ky5' defects) because of its availability as a single crystal heteroepitaxial thin film grown on silicon, an advantage that greatly facilitates the fabrication of functional devices. We characterized the spin and optical properties of Ky5 defects in thin film geometries and observed many similarities to the nitrogen vacancy center. We performed the first measurements of spin dynamics in 3C silicon carbide and demonstrate coherent control of defect spins up to room temperature and observe coherence times of up to 22 microseconds. To demonstrate their use in real devices, we designed, fabricated, and characterized photonic crystal cavities in 3C silicon carbide thin films with mode volumes of less than (lambda/n)^3 and Q's as high as 1,500 with integrated Ky5 defects. Additionally, we performed simulations and analysis of the fabricated structures using observed structural imperfections to determine that the Q's are likely limited primarily by the non-vertical structure sidewall angle. Despite the modest Q's of these structures, they can be utilized to generate large local field intensities to enhance optical interactions with Ky5 qubit states within the cavities. We accomplish this by performing cavity enhanced photoluminescence excitation spectroscopy on cavity modes tuned to the zero phonon line of the defects and observe large (as high as 30 times) increases in the luminescence and optically detected magnetic resonance signals originating from the defect states and approximately 2x faster rates of ground state spin initialization. In addition, we use these techniques to probe the photoluminescence dynamics of the Ky5 defects' optical pumping cycle, perform excitation wavelength dependent studies of spin and spectral inhomogeneity, and use the small mode volume and narrowband photoluminescence enhancements of the cavities to observe spectrally distinct subensembles of defects with linewidths as narrow as 25 GHz within the inhomogeneously broadened zero phonon line. Although much is still unknown regarding the properties of these defects, they show great promise as a candidate system for defect qubit based quantum devices and technologies.
This extension method advances the characterization of NV centers in silicon carbide (SiC) by incorporating optimization strategies, machine learning (ML), error correction, and advanced sensing protocols. While the base method validated NV centers in 4H-SiC and 6H-SiC as promising solid-state qubits, our extension aims to enhance their performance and scalability for quantum technologies. First, we identified an optimal NV ensemble density of 1.0 × 10¹⁶ cm⁻3, balancing signal strength with minimized dipole–dipole interactions, thereby maximizing collective coherence. Second, a machine learning framework was developed to optimize experimental conditions, scanning laser power, excitation wavelength, and temperature to improve phase coherence time (T₂) by nearly two-fold. Third, advanced quantum sensing protocols were benchmarked, including Ramsey, Spin-Echo, CPMG, XY-8, and ML-optimized pulse sequences, achieving up to 3.5× higher sensitivity compared to conventional spin-echo. Fourth, dynamical decoupling (N=16) was applied to mitigate decoherence, extending T₂ up to ~60 μs at room temperature. Finally, error correction simulations at the NV ensemble level demonstrated logical error rate reductions by nearly two orders of magnitude, showcasing fault-tolerance potential. Overall, this extension transforms NV–SiC centers from characterized quantum defects into a practical platform with enhanced coherence, improved sensing capabilities, and integrated error correction. These results position SiC NV ensembles as a scalable candidate for next-generation quantum computing
Silicon carbide (SiC) in its various structural modifications is widely used in power semiconductor electronics, operating under extreme conditions of high temperature, high voltage, and intense radiation. The discovery of spin defects (S>0) with unique optical and coherent properties has further positioned SiC as a promising platform for quantum technologies. Here, we investigate a 6H-SiC single crystal co-doped with nitrogen and beryllium at concentrations of 1018 cm-3, using continuous-wave and pulsed electron paramagnetic resonance (EPR) and electron-nuclear double resonance (ENDOR). To enhance spectral resolution, experiments were conducted in the W-band (94 GHz; B = 3.4 T). Pulsed EPR identified nitrogen donors and beryllium acceptors in various lattice positions, allowing for the determination of their phase coherence and spin-lattice relaxation times. ENDOR measurements elucidated the electron-nuclear interactions with the local silicon and carbon environment, including distant coordination spheres. The observed hyperfine structures indicated highly delocalized spin density within the supercell. The TRIPLE resonance spectra verify coupled nuclear spin subspaces from different coordination spheres due to defect spin density. These results demonstrate the feasibility of incorporating dual impurities with distinct functional roles while preserving the crystal lattice`s structural features.
Solid-state spin defects are a promising platform for quantum networks. A key requirement is to combine long ground-state spin-coherence times with a coherent optical transition for spin-photon entanglement. Here, we investigate the spin and optical coherence of single nitrogen-vacancy (NV) centres in (111)-grown isotopically engineered diamond. Our diamond-growth process yields a precisely controlled 13C^{13}\mathrm{C}13C concentration and low-ppb nitrogen concentrations. Combined with the mitigation of 50 Hz noise using a real-time feedforward scheme and tailored decoupling sequences, this enables record defect-electron-spin coherence times of T2=6.8(1)T_2 = 6.8(1)T2​=6.8(1) ms for a Hahn echo and of T2DD=11.2(8)T_2^{DD} = 11.2(8)T2DD​=11.2(8) s under dynamical decoupling. In addition, we observe coherent optical transitions with a near-lifetime-limited homogeneous linewidth of 16.9(4) MHz and characterize the spectral diffusion dynamics. These results provide new avenues to investigate the incorporation of impurities in diamond and new opportunities for improved spin-qubit control for quantum networks and other quantum technologies.