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Light Science & Applications

Spin-manipulated nanoscopy for single nitrogen-vacancy center localizations in nanodiamonds

Martina Barbiero, Stefania Castelletto, Xiaosong S. Gan, Miṅ Gu

Published May 10, 2017• 29 citations
Publisher

Abstract

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.

DOI
10.1038/lsa.2017.85

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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.
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.
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.
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.
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.
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.