Solid Immersion Facilitates Fluorescence Microscopy with Nanometer Resolution and Sub‐Ångström Emitter Localization

Wildanger, Dominik; Patton, Brian; Schill, Heiko; Marseglia, Luca; Hadden, J. P.; Knauer, Sebastian; Schönle, Andreas; Rarity, John; O'Brien, Jeremy L.; Hell, Stefan W.; Smith, Jason M.

doi:10.1002/adma.201203033

Cited by 130 publications

(105 citation statements)

References 23 publications

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“…22 To further improve the spatial resolution, a high numerical aperture oil objective could be used in the future. Such an objective would produce a higher charge-state conversion rate gradient than a dry objective.…”

Section: Csd Microscopymentioning

confidence: 99%

“…With STED, the electron spin resonance signals of NV centers have been detected with a resolution lower than the diffraction limit. 12,21,22 A new super-resolution microscopy technique was recently developed by Han et al 15 The authors replaced the stimulated excitation of STED with the dark-state pumping of NV centers. The dark state was later proven to be the neutral charge NV center (NV 0 ) by other groups.…”

Section: Introductionmentioning

confidence: 99%

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Subdiffraction optical manipulation of the charge state of nitrogen vacancy center in diamond

et al. 2015

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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. Keywords: charge state; NV center; photon ionization; super-resolution microscopy INTRODUCTION Because of the stable fluorescence and long coherence time of its spin state, the negatively charged nitrogen vacancy (NV 2 ) center in diamond has been studied extensively over the past decade. This defect has the potential to be used for quantum computation, 1-4 nanoscale metrology 5-8 and biological imaging. [9][10][11] To further extend the study of the interaction between a multi-NV center and the nanoscale sensing with the NV center, it is necessary to detect and control the NV center spin-state dynamics with high spatial resolution. 7,12-14 Therefore, many optical super-resolution microscopy techniques have been developed to detect single NV centers. [13][14][15][16][17] Among these methods, stimulated emission depletion (STED) microscopy 12,18-20 is one of the most promising. This method utilizes a doughnut-shaped laser to produce the position-dependent stimulated emission, which changes the fluorescence signal. With STED, the electron spin resonance signals of NV centers have been detected with a resolution lower than the diffraction limit. 12,21,22 A new super-resolution microscopy technique was recently developed by Han et al. 15 The authors replaced the stimulated excitation of STED with the dark-state pumping of NV centers. The dark state was later proven to be the neutral charge NV center (NV 0 ) by other groups. [23][24][25] The charge-state conversion results in a change of the local field in diamond 26 and the spectral diffusion of the NV center. 24,27 For high-fidelity quantum manipulation, the charge state should be well controlled. 28 Based on the mechanism of charge-state conversion and super-resolution microscopy, 25,29,30 we demonstrated the optical manipulation of the charge state of an NV center with subdiffraction resolution. By changing the duration and power of laser

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Section: Csd Microscopymentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Subdiffraction optical manipulation of the charge state of nitrogen vacancy center in diamond

et al. 2015

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“…In bulk diamond, record resolutions down to 6 nm 5 were achieved, and in conjunction with solid immersion, a resolving power of 2.4 nm 6 was demonstrated, corresponding to 1/323 of the applied wavelength. However, the task to individually resolve NV centers located inside diamond crystals of subwavelength dimensions (i.e., nanodiamonds) by means of STED microscopy has not yet been demonstrated, 7,8 nourishing speculations about whether it is possible at all.…”

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confidence: 99%

Stimulated Emission Depletion Microscopy Resolves Individual Nitrogen Vacancy Centers in Diamond Nanocrystals

et al. 2013

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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 superresolution 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 40À250 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 À spins inside nanodiamonds by STED should also be of high significance for quantum sensing and information applications.

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“…STED can resolve much more sophisticated details (Figure 7a) than the confocal microscope (Figure 7b), for example, the published resolution record of 2.4 nm was just achieved in 2012. 58 Dynamic imaging with a frame rate as high as 200 fps has been reported 59 for this method, and it is also possible to realize multi-color imaging and 3D nanoscale reconstruction. 60 The theoretical resolution of a STED microscope can be expressed as: 61 …”

Section: Absolute Far-field Strategiesmentioning

confidence: 99%

From microscopy to nanoscopy via visible light

Hao

Kuang

et al. 2013

Light Sci Appl

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The resolution of conventional optical equipment is always restricted by the diffraction limit, and improving on this was previously considered improbable. Optical super-resolution imaging, which has recently experienced rapid growth and attracted increasing global interest, will result in applications in many domains, benefiting fields such as biology, medicine and material research. This review discusses the contributions of different researchers who identified the diffractive barrier and attempted to realize optical super-resolution. This is followed by a personal viewpoint of the development of optical nanoscopy in recent decades and the road towards the next generation of optical nanoscopy.

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Solid Immersion Facilitates Fluorescence Microscopy with Nanometer Resolution and Sub‐Ångström Emitter Localization

Cited by 130 publications

References 23 publications

Subdiffraction optical manipulation of the charge state of nitrogen vacancy center in diamond

Subdiffraction optical manipulation of the charge state of nitrogen vacancy center in diamond

Stimulated Emission Depletion Microscopy Resolves Individual Nitrogen Vacancy Centers in Diamond Nanocrystals

From microscopy to nanoscopy via visible light

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