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Conference on Lasers and Electro-Optics

Super-resolution magnetic imaging of magnetic nanoparticles with charge state depletion of nitrogen vacancy centers in diamond

Nazanin Mosavian, Forrest Hubert, Jānis Šmits, Pauli Kehayias, Yaser Silani, Nathaniel Ristoff, Bryan Richards, Víctor M. Acosta

Published Jan 1, 2022• 1 citation
Publisher

Abstract

We have used a method called Charge State Depletion (CSD) microscopy with Nitrogen-Vacancy (NV) centers in diamond to perform fluorescence microscopy beyond the diffraction limit. Combined with Optically Detected Magnetic Resonance (ODMR) measurements on NV centers in a layer near the diamond surface, this enables super-resolution magnetic microscopy of ~30 nm ferromagnetic nanoparticles.

DOI
10.1364/cleo_at.2022.jth3a.30

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•Jan 1, 2018•0 citations
We have used a method called Charge State Depletion (CSD) microscopy with Nitrogen-Vacancy (NV) centers in diamond to perform fluorescence microscopy beyond the diffraction limit. Combined with Optically Detected Magnetic Resonance (ODMR) measurements on NV centers in a layer near the diamond surface, this enables super-resolution magnetic microscopy of ~30 nm ferromagnetic nanoparticles.
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.
As a potential candidate for quantum computation and metrology, the nitrogen vacancy (NV) center in diamond presents both challenges and opportunities resulting from charge-state conversion. By utilizing different lasers for the photon-induced charge-state conversion, we achieved subdiffraction charge-state manipulation. The charge-state depletion (CSD) microscopy resolution was improved to 4.1 nm by optimizing the laser pulse sequences. Subsequently, the electron spin-state dynamics of adjacent NV centers were selectively detected via the CSD. The experimental results demonstrated that the CSD can improve the spatial resolution of the measurement of NV centers for nanoscale sensing and quantum information. The nitrogen vacancy (NV) in diamond is useful for quantum optics and spintronics due to the long coherence time of its electron spin state. Scientists in China have now used the techniques of super-resolution microscopy to optically control the charge state of an NV defect with a subdiffraction spatial resolution of 4.1 nm. Xiangdong Chen and co-workers from the University of Science and Technology of China in Hefei used a green (532 nm) laser beam to switch the charge state of the defect between NV0 and NV–. They achieved this manipulation on a subdiffraction scale by using specially shaped doughnut laser beams, in common with the principles of super-resolution stimulated emission depletion microscopy. This achievement represents a significant step towards nanoscale sensing and quantum information processing.
Nitrogen-vacancy (NV) color centers in nanodiamonds are highly promising for bioimaging and sensing. However, resolving individual NV centers within nanodiamond particles and the controlled addressing and readout of their spin state has remained a major challenge. Spatially stochastic super-resolution techniques cannot provide this capability in principle, whereas coordinate-controlled super-resolution imaging methods, like stimulated emission depletion (STED) microscopy, have been predicted to fail in nanodiamonds. Here we show that, contrary to these predictions, STED can resolve single NV centers in 40-250 nm sized nanodiamonds with a resolution of ≈10 nm. Even multiple adjacent NVs located in single nanodiamonds can be imaged individually down to relative distances of ≈15 nm. Far-field optical super-resolution of NVs inside nanodiamonds is highly relevant for bioimaging applications of these fluorescent nanolabels. The targeted addressing and readout of individual NV(-) spins inside nanodiamonds by STED should also be of high significance for quantum sensing and information applications.
Fluorescent nitrogen vacancies (NV) in diamond have drawn much interest because of their potential for computation and quantum cryptography, as well as for nanoscale magnetic imaging and biolabeling due to their special spin and fluorescence properties. However, their optical detection and control is compromised by the diffraction resolution barrier of far-field optics. We showed that stimulated emission depletion (STED) microscopy is capable of imaging NV centres with nanoscale resolution and Ångström precision using focused visible light [1].
Due to their exceptional optical and magnetic properties, negatively charged nitrogen-vacancy (NV−) centers in nanodiamonds (NDs) have been identified as an indispensable tool for imaging, sensing and quantum bit manipulation. The investigation of the emission behaviors of single NV− centers at the nanoscale is of paramount importance and underpins their use in applications ranging from quantum computation to super-resolution imaging. Here, we report on a spin-manipulated nanoscopy method for nanoscale resolutions of the collectively blinking NV− centers confined within the diffraction-limited region. Using wide-field localization microscopy combined with nanoscale spin manipulation and the assistance of a microwave source tuned to the optically detected magnetic resonance (ODMR) frequency, we discovered that two collectively blinking NV− centers can be resolved. Furthermore, when the collective emitters possess the same ground state spin transition frequency, the proposed method allows the resolving of each single NV− center via an external magnetic field used to split the resonant dips. In spin manipulation, the three-level blinking dynamics provide the means to resolve two NV− centers separated by distances of 23 nm. The method presented here offers a new platform for studying and imaging spin-related quantum interactions at the nanoscale with super-resolution techniques. A new spin-manipulated nanoscopy method can resolve collectively blinking negatively charged nitrogen-vacancy centers (NVCs) on a nanoscale. The exceptional optical and magnetic properties of negatively charged nitrogen-vacancy centers in nanodiamonds make them attractive as fluorescent biomarkers in imaging and sensing applications. By combining wide-field localization microscopy with nanoscale spin manipulation by a microwave signal, Min Gu and colleagues from RMIT University and Swinburne University of Technology in Australia have achieved super-resolution imaging of the blinking of multiple, closely spaced negatively charged NVCs. The nanoscopy approach can resolve NVCs as small as 42 nanometers and separated by as little as 23 nanometers. Two close NVCs often appear to emit coupled fluorescence as they exhibit a collective behavior. The method offers a new way to study and image spin-related quantum interactions at the nanoscale.
The NV defect center in diamond forms a pseudo-atomic quantum system with discreet optically excitable transitions between ground and excited states in the gap between valence and conduction bands, making the NV center a deep-level defect center in diamond. For the negatively charged NV center (NV-), both the ground and excited states are spin triplets (S=1) and coupling between optical and spin states provides unique opportunities for optical detection of magnetic resonance (ODMR) and quantum metrology under ambient conditions. As an atomically sized point defect that is stable in single nanodiamonds as small as a few nanometers, the NV center enables spin based imaging of temperature, electric fields, magnetic fields and mechanical strain with nanoscale spatial resolution. Made of carbon, nanodiamonds are also ideal nanoparticles for use in biological systems, exhibiting extremely low cytotoxicity, no photo bleaching and exceptional contrast in transmission electron and light microscopy. With the ability to act as both a passive, non perturbing sensor (e.g. a diamagnetic material used for sensing magnetic fields) and a connection point for two way, direct coupling of far field optics to NV−^-− spins and indirectly to the highly localized neighborhood of atoms, electronic states and phonon modes in the local vicinity, NV diamond provides a route to nanoscale field sensing and spin based optical microscopy. These sensors are also stable in nanodiamonds. For nanoparticles, the reduction in particle diameter dramatically enhances the proportion of the material that is surface exposed, enhancing any surface related properties. Nitrogen Vacancy centers in nanodiamonds provide another example of material properties that vary with particle size. In chapter 5, evidence that modulation of nanodiamonds fluorescent emissions by electrical perturbations in their surrouding environment allows transduction of local electrodynamics into a far field optical signal capable of mapping action potentials in cardiomyocytes in presented. The unifying theme for all of the work presented in this dissertation is to enable the use of magnetic resonance signals and interactions for imaging and sensing in previously inaccessible regimes. The specific focus is on methods and techniques to enable nanoscale physical sensing and functional imaging in live tissues, with the ultimate aim to lay the predicate for the combination of both without compromise.