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Advanced Science

Multimodal Super‐Resolution Imaging of Nitrogen‐Vacancy Centers via High‐Index‐Induced Structured Illumination Microscopy and Optically Detected Magnetic Resonance Spectrometry

Kyu Ri Choi, Mohammed Zia Jalaludeen, Samuel Begumya, Yan Qiu Du, Dong Hee Park, Bin Chan Joo, Jae Hwan Yoo, Síle Nic Chormaic, Shilong Li, Yeon Ui Lee

Published Mar 3, 2026• 0 citations
Publisher

Abstract

Structured illumination microscopy (SIM) allows for optical imaging with spatial resolution that surpasses the diffraction limit. To further enhance this super-resolution capability, we present a multimodal approach that integrates SIM with optically detected magnetic resonance (ODMR) of nitrogen-vacancy (NV) centers in diamond-a platform considered one of the most promising platforms for quantum sensing and computing. Both theoretical modeling and experimental results reveal that diamond's high refractive index supports finer structured illumination patterns, thereby accessing higher spatial frequencies and yielding improved resolution. This combined strategy not only enhances NV center localization precision and achieves sub-100-nm resolution but also facilitates spin coherence analysis. Leveraging the high refractive index of diamond in SIM thus offers a powerful pathway toward advancing quantum applications at the nanoscale.

DOI
10.1002/advs.202522495

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Structured illumination microscopy (SIM) allows for optical imaging with spatial resolution that surpasses the diffraction limit. To further enhance this super-resolution capability, we present a multimodal approach that integrates SIM with optically detected magnetic resonance (ODMR) of nitrogen-vacancy (NV) centers in diamond-a platform considered one of the most promising platforms for quantum sensing and computing. Both theoretical modeling and experimental results reveal that diamond's high refractive index supports finer structured illumination patterns, thereby accessing higher spatial frequencies and yielding improved resolution. This combined strategy not only enhances NV center localization precision and achieves sub-100-nm resolution but also facilitates spin coherence analysis. Leveraging the high refractive index of diamond in SIM thus offers a powerful pathway toward advancing quantum applications at the nanoscale.
Wide-field quantum sensing and imaging with solid-state spins has attracted wide interest for its ability to detect relative physical quantities with high sensitivity at nanoscale. However, the optical diffraction limit hinders the improvement in spatial resolution. In this work, we utilize blind structured illumination microscopy to perform wide-field quantum sensing with nitrogen-vacancy (NV) center in diamond. Without the requirement of prior knowledge of excitation light field, the spatial resolution of NV centers imaging is enhanced by 1.8-fold in comparison with conventional microscopy. Combined with spin manipulation and detection, super-resolution NV center sensing is subsequently performed to reveal the optical and electrical properties of nanodevice. The high spatial resolution and feasibility of this work will promote the applications of quantum sensing in nanoscience.
Nitrogen vacancy (NV) color centers in diamond are a leading modality for both superresolution optical imaging and nanoscale magnetic field sensing. In this work, we address the key challenge of performing optical magnetic imaging and spectroscopy selectively on multiple NV centers that are located within a diffraction-limited field-of-view. We use spin-RESOLFT microscopy to enable precision nanoscale mapping of magnetic field patterns with resolution down to ~20 nm, while employing a low power optical depletion beam. Moreover, we use a shallow NV to demonstrate the detection of proton nuclear magnetic resonance (NMR) signals exterior to the diamond, with 50 nm lateral imaging resolution and without degrading the proton NMR linewidth.
Quantum sensing using nitrogen-vacancy (NV) centers in diamond has emerged as a powerful platform for detecting ultra-low magnetic fields under ambient conditions. Owing to their long spin coherence times, optical addressability, and compatibility with aqueous environments, it has found widespread applications in biosensing and bio-imaging. This review presents the fundamental principles and recent advances in NV-based quantum magnetometry for biosensing applications, with a particular focus on measurements in aqueous medium and at cellular and molecular length scales. We discuss the underlying spin physics of NV centers and highlight two primary detection modalities: optically detected magnetic resonance (ODMR) and T1 relaxometry-based sensing and how these approaches aids in the detection of both static magnetic fields and dynamic magnetic noise arising from biological processes. The review explores key application areas, including nanoscale nuclear magnetic resonance (NMR), monitoring of neural activity, detection of abnormal or rogue cells using NV-based platforms etc. In addition, strategies for enhancing sensitivity, such as surface functionalization of nanodiamonds, femtosecond (fs) laser-written photonic structures, and integration with microfluidic and lab-on-chip systems have also been discussed in depth. We also address the critical challenges, including surface-induced decoherence, charge-state instability, and signal-to-noise limitations in biofluids associated with NV-based biosensing applications. Finally, we outline future prospects, highlighting how NV-based magnetic biosensing provides a promising pathway for translating quantum sensing technologies into practical biomedical applications.
We experimentally demonstrate precision addressing of single-quantum emitters by combined optical microscopy and spin resonance techniques. To this end, we use nitrogen vacancy (NV) color centers in diamond confined within a few ten nanometers as individually resolvable quantum systems. By developing a stochastic optical reconstruction microscopy (STORM) technique for NV centers, we are able to simultaneously perform sub-diffraction-limit imaging and optically detected spin resonance (ODMR) measurements on NV spins. This allows the assignment of spin resonance spectra to individual NV center locations with nanometer-scale resolution and thus further improves spatial discrimination. For example, we resolved formerly indistinguishable emitters by their spectra. Furthermore, ODMR spectra contain metrology information allowing for sub-diffraction-limit sensing of, for instance, magnetic or electric fields with inherently parallel data acquisition. As an example, we have detected nuclear spins with nanometer-scale precision. Finally, we give prospects of how this technique can evolve into a fully parallel quantum sensor for nanometer resolution imaging of delocalized quantum correlations.
We investigated the spatial resolution of scanning photocurrent microscopy (SPhM) for imaging single nitrogen-vacancy (NV) centers in diamond in detail and compared it with that of confocal laser scanning microscopy (CLSM). While CLSM suffers from degraded spatial resolution due to fluorescence saturation, SPhM maintains a high spatial resolution despite the high-power laser excitation required. Numerical simulations of SPhM and CLSM images showed good agreement with experimental data and further indicated that SPhM achieves superior spatial resolution. Additionally, the signal-to-noise ratio of the photoelectrically detected magnetic resonance spectrum is comparable to that of the optically detected magnetic resonance spectrum in our home-made spectrometers. These findings suggest that SPhM can enhance the performance of NV-based quantum sensors.