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The Journal of Physical Chemistry C

NV Centers Coherent Behavior in 6H-SiC Crystal under Optical Nonresonant Excitation

Fadis F. Murzakhanov, Georgy Vladimirovich Mamin, Ekaterina V. Dmitrieva, I. N. Gracheva, Yuliya E. Ermakova, Marat Revgerovich Gafurov

Published Jul 4, 2025• 1 citation
Publisher

Abstract

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.

DOI
10.1021/acs.jpcc.5c03454

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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.
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.
Robust single spin color centers in solid state systems with telecom wavelength emission are vital to quantum photonics and quantum networks. The nitrogen vacancy (NV) centers in silicon carbide (SiC) have become promising platforms for those applications. However, little is known about the detailed optical properties of the NV centers. In this paper, we investigate the photophysics of the single NV centers in 4H-SiC. The results demonstrate that the NV centers comprise three energy-level electronic structures. Particularly, for c -axis NV centers, both the excitation and the emission polarization degrees are larger than 90%. Photon purity and photostability of the single NV centers are maintained at an elevated temperature up to 400 K. These experiments constitute an important step toward using the NV centers in SiC with respect to quantum photonics.
We have investigated the optical properties of the ${(\mathrm{NV})}^{\ensuremath{-}}$ center in 3C-SiC to determine the photoluminscence zero phonon line (ZPL) associated with the $^{3}\mathrm{E}\ensuremath{\rightarrow}^{3}\mathrm{A}_{2}$ intracenter transition. Combining electron paramagnetic resonance and photoluminescence spectroscopy, we show that the ${\mathrm{NV}}^{\ensuremath{-}}\phantom{\rule{0.28em}{0ex}}\mathrm{center}$ in 3C-SiC has a ZPL line at 1.468 $\ensuremath{\mu}\mathrm{m}$ in excellent agreement with theoretical predictions. The ZPL line can be observed up to T=100T=100T=100 K. The negatively charged NV center in 3C-SiC is the structural isomorphe of the NV center in diamond and has equally a spin S=1S=1S=1 ground state and a spin S=1S=1S=1 excited state, long spin lattice relaxation times and presents optically induced groudstate spin polarization. These properties make it already a strong competitor to the NV center in diamond, but as its optical domain is shifted in the near infrared at $1.5\phantom{\rule{0.16em}{0ex}}\ensuremath{\mu}\mathrm{m}$, the NV center in 3C-SiC is compatible with quantum photonic networks and silicon based microelectronics.
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 sixfold through optimization of implantation conditions. Hence, coherent control of NV center spins is achieved at room temperature, and the coherence time T_{2} can be reached to around 17.1 μs. Furthermore, an investigation of fluorescence properties of single NV centers shows that they are room-temperature photostable single-photon sources at telecom range. Taking advantage of technologically mature materials, the experiment demonstrates that the NV centers in silicon carbide are promising platforms for large-scale integrated quantum photonics and long-distance quantum networks.
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.
Silicon carbide (SiC) has become a key player in the 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 results highligh the key role of NV centers in SiC as a potential candidate for quantum information processing.