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Optics Express

Super-resolving single nitrogen vacancy centers within single nanodiamonds using a localization microscope

Miṅ Gu, Yaoyu Cao, Stefania Castelletto, Betty P. Kouskousis, Xiangping Li

Published Jul 16, 2013• 52 citations
Publisher

Abstract

In this paper, we show super-resolving single nitrogen vacancy (NV) centers with a sub-20 nanometer resolution in a wide-field localization microscope based on the discovery of photoluminescence blinking in high-pressure high-temperature nanodiamonds (NDs). The photon statistics reveals that NDs containing not only single but also multiple NV centers show photoluminescence blinking. The combination of an atomic force microscope and an optical localization microscope built on the blinking feature enables the optically resolved two NV centers within single NDs for the first time. Our method establishes new avenues for studying nanoscale photon dynamics associated with single NV centers within NDs together with ND-based ultra-sensitive bioimaging devices.

DOI
10.1364/oe.21.017639

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Optics Express•Nov 24, 2014•16 citations
In this paper, we show super-resolving single nitrogen vacancy (NV) centers with a sub-20 nanometer resolution in a wide-field localization microscope based on the discovery of photoluminescence blinking in high-pressure high-temperature nanodiamonds (NDs). The photon statistics reveals that NDs containing not only single but also multiple NV centers show photoluminescence blinking. The combination of an atomic force microscope and an optical localization microscope built on the blinking feature enables the optically resolved two NV centers within single NDs for the first time. Our method establishes new avenues for studying nanoscale photon dynamics associated with single NV centers within NDs together with ND-based ultra-sensitive bioimaging devices.
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.
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 negatively charged nitrogen-vacancy ([Formula: see text]) centre in nanodiamonds (NDs) has been recently studied for applications in cellular imaging due to its better photo-stability and biocompatibility if compared to other fluorophores. Super-resolution imaging achieving 20-nm resolution of [Formula: see text] in NDs has been proved over the years using sub-diffraction limited imaging approaches such as single molecule stochastic localisation microscopy and stimulated emission depletion microscopy. Here we show the first demonstration of ground-state depletion (GSD) nanoscopy of these centres in NDs using three beams, a probe beam, a depletion beam and a reset beam. The depletion beam at 638 nm forces the [Formula: see text] centres to the metastable dark state everywhere but in the local minimum, while a Gaussian beam at 594 nm probes the [Formula: see text] centres and a 488-nm reset beam is used to repopulate the excited state. Super-resolution imaging of a single [Formula: see text] centre with a full width at half maximum of 36 nm is demonstrated, and two adjacent [Formula: see text] centres separated by 72 nm are resolved. GSD microscopy is here applied to [Formula: see text] in NDs with a much lower optical power compared to bulk diamond. This work demonstrates the need to control the NDs nitrogen concentration to tailor their application in super-resolution imaging methods and paves the way for studies of [Formula: see text] in NDs' nanoscale interactions.
Diamond nanocrystals containing highly photoluminescent color centers are attractive, nonclassical, and near-field light sources. For near-field applications, the size of the nanocrystal is crucial, since it defines the optical resolution. Nitrogen-vacancy (NV) color centers are efficiently created by proton irradiation and annealing of a nanodiamond powder. Using near-field microscopy and photon statistics measurements, we show that nanodiamonds with sizes down to 25 nm can hold a single NV color center with bright and stable photoluminescence.
We investigated the suitability of nanodiamonds (NDs) with nitrogen-vacancy (NV) centres as samples for resolution tests in stimulated emission depletion (STED) microscopy. The nanodiamonds were prepared using three different methods including additional proton irradiation to enhance NV centre density. This high-density sample exhibited stronger photoluminescence intensity, greater fluorescence stability, and higher image contrast under STED conditions. All samples showed strong resistance to damage from high STED laser power. Our results highlight the robustness and effectiveness of NDs with NV centres as reliable standards for evaluating STED microscope resolution.
Precise positioning of nitrogen-vacancy (NV) centers is crucial for their application in sensing and quantum information. Here we present a new purely optical technique enabling determination of the NV position with nanometer resolution. We use a confocal microscope to determine the position of individual emitters along the optical axis. Using two separate detection channels, it is possible to simultaneously measure reflected light from the diamond surface and fluorescent light from the NV center and statistically evaluate both signals. An accuracy of 2.6 nm for shallow NV centers was achieved and is consistent with other techniques for depth determination.