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arXiv:1610.02097 · Optics Express

Superresolution optical magnetic imaging and spectroscopy using individual electronic spins in diamond

Jean-Christophe Jaskula, Erik Bauch, Silvia Arroyo-Camejo, Mikhail D. Lukin, Stefan W. Hell, Alexei S. Trifonov, Ronald Lee Walsworth

Published May 3, 2017• 51 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1364/oe.25.011048

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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.
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].
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.
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.
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.
High spatial resolution and low perturbation are required for mapping the electromagnetic field at the nanoscale, to provide crucial information about local light-matter interaction. Using optical superresolution microscopy for detection via a nitrogen-vacancy center in diamond, this work demonstrates far-field noninvasive sensing of the local electromagnetic field with high accuracy and a spatial resolution of approximately 50 nm. As the nitrogen-vacancy center is sensitive to various physical quantities, a multifunctional far-field quantum nanoscope is anticipated.