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Journal of Physics Conference Series

Saturation of fluorescence from NV centers in Mie-resonant diamond particles

Dmitry V. Obydennov, Шилкин Даниил Александрович, Evgeny V. Lyubin, Maxim R. Shcherbakov, Evgeny F. Ekimov, Oleg S. Kudryavtsev, Igor I. Vlasov, Andrey A. Fedyanin

Published Sep 1, 2018• 2 citations
Publisher

Abstract

Diamond particles with color centers have found numerous applications in quantum optics, bioimaging and nanosensing. Here, we report on an experimental study of the optical Mie resonances of subwavelength diamond particles and their effect on the fluorescence of nitrogen-vacancy centers. We employ single-particle scattering spectroscopy to reveal the fundamental optical resonances of individual diamond particles and measure the fluorescence saturation curves using continuous-wave excitation to evidence the difference in the spontaneous emission rate of the color centers in different particles. A simple analytical model has been used to predict the dependence of the saturation intensity on the particle size for a free-standing spherical diamond. Experimentally, we have shown that the magnetic dipole and quadrupole modes are excited in the fluorescence spectral range for particles of approximately 250-350 nm in size and that the saturation intensity for such particles is by an order of magnitude higher than for a smaller one, which is in agreement with our calculations. The results demonstrate that the efficiency of diamond-based sensors and single-photon sources can be improved by simply choosing particles of a proper size.

DOI
10.1088/1742-6596/1092/1/012102

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Diamond particles with color centers have found numerous applications in quantum optics, bioimaging and nanosensing. Here, we report on an experimental study of the optical Mie resonances of subwavelength diamond particles and their effect on the fluorescence of nitrogen-vacancy centers. We employ single-particle scattering spectroscopy to reveal the fundamental optical resonances of individual diamond particles and measure the fluorescence saturation curves using continuous-wave excitation to evidence the difference in the spontaneous emission rate of the color centers in different particles. A simple analytical model has been used to predict the dependence of the saturation intensity on the particle size for a free-standing spherical diamond. Experimentally, we have shown that the magnetic dipole and quadrupole modes are excited in the fluorescence spectral range for particles of approximately 250-350 nm in size and that the saturation intensity for such particles is by an order of magnitude higher than for a smaller one, which is in agreement with our calculations. The results demonstrate that the efficiency of diamond-based sensors and single-photon sources can be improved by simply choosing particles of a proper size.
The resonant high-index nanostructures open opportunities for control many optical effects via optically-induced electric and magnetic Mie resonances, mostly localized inside the structures. Especial interest such nanostructures represent for quantum emitters placed inside, that makes possible enhancement of quantum source emission through resonant coupling to localized modes. We have proposed the concept of active dielectric nanoantennas based on nanodiamonds with embedded NV-centers. The study of theoretically dependence of optical properties of this system on the spectral position of the resonant modes has demonstrated that that at some sizes of the diamond spherical particles and certain position of the dipole in the sphere the Purcell factor can achieve the value of 30. We have demonstrated experimentally that the photoluminescence properties of the NV-centers can be controlled via scattering resonances and observed a decrease of the NV-centers lifetime in the studied diamond particles, as compared to nonresonant nanodiamonds. These results are in a good agreement with our theoretical calculations for the average Purcell factor for multiple NV-centers within a nanoparticle. The simplicity of the proposed concept compared to existing photonic cavity systems and applicability for a wide range of color centers in diamond make active diamond nanoantenna an effective tool for creating controllable emitting elements in the visible range for future nanophotonic devices.
We report experimental studies of microsphere-enhanced fluorescence collection of nitrogen vacancy (NV) centers using silica microspheres with diameters ranging between 15 and 50 μm and employing 20× and 40× objectives with numerical aperture of 0.42 and 0.64, respectively. Photoluminescence-excitation saturation counts as high as 95 kHz have been observed. These studies show that due to the effective collimation of fluorescence by the microsphere, objectives with relatively low numerical aperture (NA) can be used without sacrificing collection enhancement, in agreement with a theoretical model based on Mie scattering. The large enhancement of fluorescence collection with relatively low NA objectives, which feature extralong working distance and are relatively inexpensive, can potentially enable wider use of NV-based quantum sensing in real world applications.
Nitrogen–vacancy (NV) centers in diamond are generally recognized as highly promising as indefinitely stable highly efficient single-photon sources. We report an experimental quantification of the brightness, radiative decay rate, nonradiative decay rate and quantum efficiency of single NV centers in diamond nanocrystals. Our experiments show that the commonly observed large spread in fluorescence decay rates of NV centers in nanodiamond is inconsistent with the common explanation of large nanophotonic mode-density variations in the ultra-small high-index crystals at near-unity quantum efficiency. We report that NV centers in 25 nm nanocrystals are essentially insensitive to local density of optical states (LDOS) variations that we induce at a dielectric interface by using liquids to vary the refractive index, and propose that quantum efficiencies in such nanocrystals are widely distributed between 0 and 20%. For single NV centers in larger 100 nm nanocrystals, we show that decay rate changes can be reversibly induced by nanomechanically approaching a mirror to change the LDOS. Using this scanning mirror method, for the first time we report calibrated quantum efficiencies of NV centers, and show that different but nominally identical nanocrystals have widely distributed quantum efficiencies between 10 and 90%. Our measurements imply that nanocrystals that are to be assembled into hybrid photonic structures for cavity QED should first be individually screened to assess fluorescence properties in detail.
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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 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 development of reliable devices to generate single photons is crucial for applications in quantum cryptography, as well as for fundamental quantum optics experiments. Due to their extremely high photostability at room temperature, optically active defects in solids, the so called color centers, are among the most promising candidates. Single NV (nitrogen-vacancy) centers in diamond have been demonstrated to be able to generate single photons and have already shown advantages compared to attenuated laser pulses in a quantum cryptography experiment. The nitrogen-vacancy center (NV center) in diamond consists of a substitutional nitrogen atom and an adjacent vacancy. This complex exhibits an optical transition with a fluorescence lifetime of 11.6 ns. The room temperature spectrum of the NV center consists of the zero-phonon line at 637 nm and broad phononic sidebands with a FWHM of more than 100 nm. Due to the existence of a shelving level the efficiency of the NV center as a single photon source is limited. Additionally, the high diffraction index of bulk diamond restricts the efficiency to collect the fluorescence light.