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arXiv:2602.01521

Spin Relaxometry with Solid-State Defects: Theory, Platforms, and Applications

Ruotian Gong, Alex L. Melendez, Guanghui He, Zhongyuan Liu, Chong Zu, Huan Zhao

cond-mat.mes-hallquant-phSubmitted Feb 2, 2026• Announced Feb 3, 2026
v1 · Feb 2, 2026v2 · Jul 10, 2026
arXivHTMLPDF

Abstract

Spin relaxometry using solid-state spin defects, such as the diamond nitrogen-vacancy (NV) center, probes dynamical processes by measuring how environmental fluctuations enhance the spin relaxation rate. In the weak-coupling limit, relaxation rates sample the transverse magnetic-noise power spectral density through a sensor-specific filter function, turning the defect into a local, frequency-selective noise spectrometer. This review bridges theory and experiment, clarifying how measured relaxation rates map onto noise spectra and how near-field geometry shapes the response. We highlight representative applications across condensed-matter physics, chemical and biological sensing, and relaxometry-based magnetic-resonance spectroscopy. We conclude with emerging opportunities and key challenges.

Comments
19 pages, 5 figures

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IntechOpen eBooks•Feb 8, 2021•1 citation
Spin relaxometry using solid-state spin defects, such as the diamond nitrogen-vacancy (NV) center, probes dynamical processes by measuring how environmental fluctuations enhance the spin relaxation rate. In the weak-coupling limit, relaxation rates sample the transverse magnetic-noise power spectral density through a sensor-specific filter function, turning the defect into a local, frequency-selective noise spectrometer. This review bridges theory and experiment, clarifying how measured relaxation rates map onto noise spectra and how near-field geometry shapes the response. We highlight representative applications across condensed-matter physics, chemical and biological sensing, and relaxometry-based magnetic-resonance spectroscopy. We conclude with emerging opportunities and key challenges.
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Quantum relaxometry is one of the most successful applications of nitrogen-vacancy (NV) centers in diamond and, more broadly, solid-state spin qubits, enabling ultrasensitive detection of magnetic noise and paramagnetic species via measurements of the spin-lattice relaxation time T1T_1T1​. Conventional pulsed protocols, however, probe T1T_1T1​ efficiently only over a limited temporal range, which restricts the scope and throughput of the technique. Here we introduce a continuous-wave quantum relaxometry protocol that operates in the frequency domain. By measuring the frequency response of the optically detected magnetic resonance signal under low-frequency microwave amplitude modulation, we extract T1T_1T1​ from the characteristic response time of the spin system. The method enables efficient T1T_1T1​ measurements spanning more than three orders of magnitude -- directly demonstrated from 60 μμμs to 200 ms in our experiments -- across a broad temperature range and under substantial ensemble inhomogeneity. We further show that this protocol enables quantitative relaxometry-based sensing in nanodiamonds, achieving a substantial speed-up over the pulsed methods and offering a practical approach to optimizing nanodiamond size for enhanced sensitivity.
Optically addressable solid-state spin defects have emerged as powerful multimodal quantum sensors, with nitrogen-vacancy (NV) centers in bulk diamond providing benchmark quantum control and sensitivity under ambient conditions. Embedding such defects in nanodiamonds (NDs) extends these capabilities to mobile probes capable of accessing complex biological and nanoscale environments. Reduced dimensions, however, introduce constraints beyond volumetric spin impurities, notably enhanced lattice strain and surface-induced noise sources, which shorten NV spin relaxation times (T1 and T2) and destabilize the NV charge state, as well as resulting in pronounced particle-to-particle variability in NDs typically produced by top-down approaches. These effects complicate both sensing performance and the quantitative interpretation of multimodal signals in realistic environments. This article provides a structured perspective on the physical mechanisms by which material properties constrain NV behavior in NDs, together with mitigation strategies that shape the robust use of these mobile quantum sensors for biosensing and nanoscale science.
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Quantum relaxometry based on nitrogen-vacancy (NV) centers in diamond is an easy-to-use technique that detects magnetic noise by measuring the longitudinal relaxation of NV centers. It is favored in chemical and biological applications due to the robustness against imperfect spin control. By tuning the energy level, NV relaxometry can detect magnetic noise generated by other spins and obtain magnetic resonance spectra through cross relaxation. However, the inhomogeneous broadening of NV centers greatly limits the spectral resolution of cross-relaxation spectra. Here we demonstrate a hole-burning technique to remove the inhomogeneous broadening. We utilize a weak pump field to deplete specific NV centers during the relaxation measurement, which contribute a reverse signal in the cross-relaxation spectra with a much narrower linewidth. Our method retains the convenience and sensitivity of NV relaxometry, opening up new avenues for high-resolution magnetic resonance spectroscopy in complex scenarios.
In modern-day quantum metrology, quantum sensors are widely employed to detect weak magnetic fields or nanoscale signals. Quantum devices, exploiting quantum coherence, are inevitably connected to physical constants and can achieve accuracy, repeatability, and precision approaching fundamental limits. As a result, these sensors have shown utility in a wide range of research domains spanning both science and technology. A rapidly emerging quantum sensing platform employs atomic-scale defects in crystals. In particular, magnetometry using nitrogen-vacancy (NV) color centers in diamond has garnered increasing interest. NV systems possess a combination of remarkable properties, optical addressability, long coherence times, and biocompatibility. Sensors based on NV centers excel in spatial resolution and magnetic sensitivity. These diamond-based sensors promise comparable combination of high spatial resolution and magnetic sensitivity without cryogenic operation. The above properties of NV magnetometers promise increasingly integrated quantum measurement technology, as a result, they have been extensively developed with various protocols and find use in numerous applications spanning materials characterization, nuclear magnetic resonance (NMR), condensed matter physics, paleomagnetism, neuroscience and living systems biology, and industrial vector magnetometry. In this chapter, NV centers are explored for magnetic sensing in a number of contexts. In general, we introduce novel regimes for magnetic-field probes with NV ensembles. Specifically, NV centers are developed for sensitive magnetometers for applications where microwaves (MWs) are prohibitively invasive and operations need to be carried out under zero ambient magnetic field. The primary goal of our discussion is to improve the utility of these NV center-based magnetometers.