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arXiv:2603.07265

A defect in diamond with millisecond-scale spin relaxation time at room temperature

Sounak Mukherjee, Anran Li, Johannes Eberle, Sean Karg, Zi-Huai Zhang, Mayer M. Feldman, Yilin Chen, Mark E. Turiansky, Mengen Wang, Yogendra Limbu, Tharnier O. Puel, Yueguang Shi, Matthew L. Markham, Rajesh L. Patel, Patryk Gumann, Michael E. Flatte, Chris G. Van de Walle, Stephen A. Lyon, Nathalie P. de Leon

cond-mat.mtrl-sciquant-phSubmitted Mar 7, 2026• Announced Mar 10, 2026
arXivHTMLPDF

Abstract

Spin defects in diamond are promising platforms for quantum sensing. The longest electron spin relaxation times ($T_1$) at room temperature for solid-state defects are observed in nitrogen vacancy centers in diamond, which can reach 6.67 ms, and substitutional nitrogen ("P1 centers") in diamond, which exhibit a $T_1$ of 2 ms. No other solid-state defect has exhibited millisecond-scale spin relaxation times at room temperature thus far. Here, we characterize the spin properties of the WAR5 defect in diamond with pulsed electron spin resonance. The observed $T_1$ is one of the longest for solid-state spin defects: 0.97(27) ms at room temperature and 14.38(19) min at 4 K. The observed coherence time ($T_2$) is 246(7) $μ$s, which can be extended to 6.49(34) ms at 4 K with dynamical decoupling. Furthermore, we demonstrate optical spin polarization with a range of wavelengths from 405 nm to 500 nm and propose potential zero-phonon line candidates.

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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.
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 (T1 and T2). Results show that this system provides at least two readily accessible qubits that can be used in quantum protocols even at room temperature.
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.
We demonstrate optical spin polarization of the neutrally charged silicon-vacancy defect in diamond (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 nonzero at below-resonant energies. We measure an ensemble spin coherence time T_{2}>100 μs at low-temperature, and a spin relaxation limit of T_{1}>25 s. Optical spin-state initialization around 946 nm allows independent initialization of SiV^{0} and NV^{-} within the same optically addressed volume, and SiV^{0} emits within the telecoms down-conversion band to 1550 nm: when combined with its high Debye-Waller factor, our initial results suggest that SiV^{0} is a promising candidate for a long-range quantum communication technology.
Nitrogen-vacancy (NV) color centers in diamond are excellent quantum sensors possessing high sensitivity and nano-scale spatial resolution. Their integration in photonic structures is often desired, since it leads to an increased photon emission and also allows the realization of solid-state quantum technology architectures. Here, we report the fabrication of diamond nano-pillars with diameters up to 1000 nm by electron beam lithography and inductively coupled plasma reactive ion etching in nitrogen-rich diamonds (type Ib) with [100] and [111] crystal orientations. The NV centers were created by keV-He ion bombardment and subsequent annealing, and we estimate an average number of NVs per pillar to be 4300 ± 300 and 520 ± 120 for the [100] and [111] samples, respectively. Lifetime measurements of the NVs’ excited state showed two time constants with average values of τ1 ≈ 2 ns and τ2 ≈ 8 ns, which are shorter as compared to a single color center in a bulk crystal (τ ≈ 10 ns). This is probably due to a coupling between the NVs as well as due to interaction with bombardment-induced defects and substitutional nitrogen (P1 centers). Optically detected magnetic resonance measurements revealed a contrast of about 5% and average coherence and relaxation times of T2 [100] = 420 ± 40 ns, T2 [111] = 560 ± 50 ns, and T1 [100] = 162 ± 11 μs, T1 [111] = 174 ± 24 μs. These pillars could find an application for scanning probe magnetic field imaging.
Nitrogen-vacancy (NV) centers in single-crystal CVD diamond are promising candidates for quantum sensing due to their remarkable optical and spin properties [1]. These defects exhibit stable photoluminescence (PL), long spin coherence times, and high sensitivity to external fields [2]. In this study, we present a room-temperature PL characterization of NV centers excited with a 532 nm laser. The setup was optimized for high signal-to-noise ratio and spectral resolution. Key parameters analyzed include emission intensity, zero-phonon line (ZPL) at ~637 nm, phonon sidebands, and the charge state distribution between NV⁰ and NV⁻. The NV⁻ state, crucial for spin-based sensing, is evaluated to understand its stability under different nitrogen doping conditions [3]. The relative intensities of NV⁰ and NV⁻ provide insights into nitrogen incorporation and vacancy formation. These results contribute to optimizing synthesis conditions for enhanced NV⁻ concentration, supporting the advancement of diamond-based quantum sensing technologies.