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Science Advances

Solid-state spin coherence time approaching the physical limit

Shuo Han, Xiangyu Ye, Xu Zhou, Zhaoxin Liu, Yuhang Guo, Mengqi Wang, Wentao Ji, Ya Wang, Jiangfeng Du

Published Feb 28, 2025• 17 citations
Publisher

Abstract

Extending the coherence time of quantum systems to their physical limit is a long-standing pursuit and critical for developing quantum science and technology. By characterizing all the microscopic noise sources of the electronic spin [nitrogen-vacancy (NV) center] in diamonds using complete noise spectroscopy, we observe a previously unforeseen noise spectrum manifested as the empirical limit ( T 2 ≈ 1 2 T 1 ) that has puzzled researchers for decades in various solid-state systems. By implementing a corresponding dynamical decoupling strategy, we are able to surpass the empirical limit and approach the upper physical limit T 2 = 2 T 1 for NVs, from room temperature down to 220 kelvin. Our observations, including the independence across different spatial sites and its dependence on temperature in the same way as spin-lattice relaxation, suggest an emerging decoherence mechanism dominated by spin-lattice interaction. These results provide a unified and universal strategy for characterizing and controlling microscopic noises, thereby paving the way for achieving the physical limit in various solid-state systems.

DOI
10.1126/sciadv.adr9298

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Extending the coherence time of quantum systems to their physical limit is a long-standing pursuit and critical for developing quantum science and technology. By characterizing all the microscopic noise sources of the electronic spin [nitrogen-vacancy (NV) center] in diamonds using complete noise spectroscopy, we observe a previously unforeseen noise spectrum manifested as the empirical limit ( T 2 ≈ 1 2 T 1 ) that has puzzled researchers for decades in various solid-state systems. By implementing a corresponding dynamical decoupling strategy, we are able to surpass the empirical limit and approach the upper physical limit T 2 = 2 T 1 for NVs, from room temperature down to 220 kelvin. Our observations, including the independence across different spatial sites and its dependence on temperature in the same way as spin-lattice relaxation, suggest an emerging decoherence mechanism dominated by spin-lattice interaction. These results provide a unified and universal strategy for characterizing and controlling microscopic noises, thereby paving the way for achieving the physical limit in various solid-state systems.
Understanding the limits to the spin coherence of the nitrogen-vacancy (NV) center in diamond is vital to realizing the full potential of this quantum system.We show that relaxation on the |m s = -1 ↔ |m s = +1 transition occurs approximately twice as fast as relaxation on the |m s = 0 ↔ |m s = ±1 transitions under ambient conditions in native NVs in high-purity bulk diamond.The rates we observe are independent of NV concentration over four orders of magnitude, indicating they are limited by spin-phonon interactions.We find that the maximum theoretically achievable coherence time for an NV at 295 K is limited to 6.8(2) ms.Finally, we present a theoretical analysis of our results that suggests Orbach-like relaxation from quasilocalized phonons or contributions due to higher-order terms in the spin-phonon Hamiltonian are the dominant mechanism behind |m s = -1 ↔ |m s = +1 relaxation, motivating future measurements of the temperature dependence of this relaxation rate.
Abstract Nitrogen-vacancy (NV) centers in diamond have been developed into essential hardware units for a wide range of solid-state-based quantum technology applications. While such applications require the long spin coherence times of the NV centers, they are often limited due to decoherence. In this study, we theoretically investigate the decoherence of NV-spin ensembles induced by nitrogen impurities (P1 centers), which are one of the most dominant and inevitable magnetic field noise sources in diamond. We combined cluster correlation expansion and density functional theory to compute the Hahn-echo spin-coherence time of the NV centers for a broad range of P1 concentrations. Results indicate a clear linear dependence of T2 on P1 concentrations on a log scale with a slope of −1.06, which is in excellent agreement with previous experimental results. The interplay between the Jahn–Teller effect and the hyperfine interaction in the P1 center plays a critical role in determining the bath dynamics and the resulting NV decoherence. Our results provide a theoretical upper bound for the NV-spin T2 over a wide range of P1 densities, serving as a key reference for materials optimization and spin bath characterization to develop highly coherent NV-based devices for quantum information technology.
The field of quantum science and technology has generated many ideas for new revolutionary devices that exploit the quantum mechanical properties of small-scale systems. Isolated solid state spins play a large role in quantum technologies. They can be used as basic building blocks for a quantum computer or as ultra-sensitive magnetic-field probes which can detect the extremely weak magnetic field generated by a single proton. A major hurdle for realizing these applications is the loss of quantum coherence resulting from uncontrolled interactions with spins in the environment. In the experiments described in my thesis we studied spins associated with defect centers in diamond and used new strategies for mitigating decoherence involving advanced quantum control techniques and for fundamental studies of decoherence. We show that we can prolong the coherence time of a single spin associated with a Nitrogen-Vacancy (NV) defect center in diamond with dynamical decoupling techniques. Our experiments are accurately reproduced theoretically and from this theory we conclude that, with dynamically decoupling, the spin environment can in principle be made irrelevant for the decoherence of a single spin. This removes a major obstacle for using solid-state spins in quantum science and technology. Furthermore, the dynamics in the spin environment and its influence on the NV spin is thoroughly experimentally studied. By better understanding the mechanisms behind decoherence we may one day find the answer to unresolved fundamental issues in quantum physics such as the quantum measurement problem.
Spin qubit coherence is a fundamental resource for the realization of quantum technologies. For solid-state platforms, spin decoherence is dominated by the magneto-active environment in the lattice, limiting their applicability. While standard dynamical decoupling techniques, such as the Hahn echo, extend central spin coherence, they fail to suppress the fast noise arising from strong dipolar interactions within the bath. Here, we present a decoupling mechanism, Hybrid-LG, that suppresses intra-bath dipolar interactions -- thus, fast noise acting on spin qubits- and demonstrate its effectiveness in extending spin coherence through efficient in-house CCE simulations. Specifically, we investigate one of the most widely exploited solid-state quantum platforms: an ensemble of nitrogen-vacancy (NV) centers in diamond coupled to a large and dense bath of substitutional nitrogen paramagnetic impurities (P1 centers). Our results reveal at least a twofold enhancement in NV coherence time relative to standard techniques including P1 center driving, without requiring additional control power.
We probe the relaxation dynamics of the full three-level spin system of near-surface nitrogen-vacancy (NV) centers in diamond to define a T_{1} relaxation time that sets the T_{2}≤2T_{1} coherence limit of the NV's subset qubit superpositions. We find that double-quantum spin relaxation via electric field noise dominates T_{1} of near-surface NVs at low applied magnetic fields. Furthermore, we differentiate 1/f^{α} spectra of electric and magnetic field noise using a novel noise-spectroscopy technique, with broad applications in probing surface-induced decoherence at material interfaces.
Abstract Nitrogen-vacancy (NV) center ensembles in diamond are one of the most promising solid-state quantum platforms for various sensing applications. Achieving ultimate sensitivity requires simultaneously long spin dephasing times ( T2∗{T}_{2}^{* }T2∗​ T 2 * ) and high NV center concentrations. In this work, we propose a systematic measurement approach to quantify the electron spin dephasing in NV center ensembles and analyze the contributions of various sources to the dephasing time, including NV-NV interactions, strain and electric field distributions, 13 C nuclear spins, and P1 electron spins. Our method is validated using a series of high-performance diamond samples, providing a comprehensive understanding of dephasing mechanisms and revealing correlations between NV concentration and different dephasing sources. Building on these insights, we outline strategies to further enhance the achievable sensitivity for DC magnetic field measurements.