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arXiv:1212.5172 · New Journal of Physics

Suitability of nanodiamond nitrogen–vacancy centers for spontaneous emission control experiments

Abbas Mohtashami, A. Femius Koenderink

Published Apr 15, 2013• 98 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1088/1367-2630/15/4/043017

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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.
Nitrogen-vacancy (NV) centers in nanodiamond are photostable single photon emitters at room temperature and are considered to be promising candidates for integrated nanophotonics and quantum information processing. A successful implementation of NV centers in nanophotonic devices requires knowledge about the photophysical properties of each emitter such as brightness, decay rate and quantum efficiency. Recent reports show that not all NV centers in diamond nanocrystals are identical and indeed show distributions in brightness and decay rate [1,2]. Here, we report on experimental quantification of the quantum efficiency (QE) of individual nanodiamonds containing single NV centers. Additionally, we report on measurements of decay rate and brightness of single nanodiamond NV centers and discuss if/which NV centers are suitable emitters to be integrated in nanophotonic devices.
The nitrogen vacancy center in diamond in its negative charge state is a promising candidate for quantum optic experiments that require single photon emitters. Important benefits of the NV center are its high brightness and photo-stability, even at room temperature. Engineering the emission properties of NV centers with optical resonators is a widely followed approach to meet the requirements for quantum technological applications, but the effect on non-radiative decay paths is yet to be understood. Here we report on modifying the internal quantum efficiency of a single NV center in a nanodiamond coupled to a 1D photonic crystal cavity. We assess the Purcell enhancement via three independent measurement techniques and perform autocorrelation measurements at elevated excitation powers in confocal microscopy. Employing a three-level model allows us to extract the setup efficiency, individual transition rates and thus the internal quantum efficiency of our system. Combining our results, we find that the enhancement of the radiative decay rate via the Purcell effect results in an internal quantum efficiency of 90 % for cavity-coupled NV centers. Our findings will facilitate the realization of nano-scale single photon sources with near-unity internal quantum efficiencies operating at high repetition rates.
The nitrogen vacancy (NV) center is the most widely studied single optical defect in diamond with great potential for applications in quantum technologies. Development of practical single-photon devices requires an understanding of the emission under a range of conditions and environments. In this work, we study the properties of a single NV center in nanodiamonds embedded in an air-like silica aerogel environment which provides a new domain for probing the emission behavior of NV centers in nanoscale environments. In this arrangement, the emission rate is governed primarily by the diamond crystal lattice with negligible contribution from the surrounding environment. This is in contrast to the conventional approach of studying nanodiamonds on a glass coverslip. We observe an increase in the mean lifetime due to the absence of a dielectric interface near the emitting dipoles and a distribution arising from the irregularities in the nanodiamond geometry. Our approach results in the estimation of the mean quantum efficiency (~0.7) of the nanodiamond NV emitters.
With in-built advantages (high quantum efficiency and room temperature photostability1) for deployment in quantum technologies as a bright on-demand source of single photons, the nitrogen vacancy (NV) center is the most widely studied optical defect in diamond. Despite significant success in controlling its spontaneous emission2, the fundamental understanding of its photo-physics in various environments and host material remains incomplete. Studying NV photoemission from nanodiamonds on a glass substrate, we recently pointed out a disparity between the measured and calculated decay rates (assuming near unity quantum efficiency)3. This indicates the presence of some strong nonradiative influences from factors most likely intrinsic to nanodiamond itself. To obtain a clearer picture of the NV emission, here we remove the substrate contributions to the decay rates by embedding our nanodiamonds inside silica aerogel, a substrate-free environment of effective index n ~ 1.05. Nanodiamond doped aerogel samples were fabricated using the “two-step” process4. Time-resolved fluorescence measurement on ~20 centers for both coverslip and aerogel configurations, showed an increase in the mean lifetime (~37%) and narrowing of the distribution width (~40%) in the aerogel environment, which we associate with the absence of a air/cover-glass interface near the radiating dipoles3. Finite difference time domain (FDTD) calculations showed the strong influence of the irregular nanodiamond geometry on the remaining distribution width. Finally a comparison between measurements and calculations provides an estimate of the quantum efficiency of the nanodiamond NV emitters as ~0.7. This value is apparently consistent with recent reports concerning the oscillation of the NV center between negative and neutral charge states5.
Spontaneous emission from crystal centers is influenced by both the photonic local density of states and non-radiative processes. Here, we monitor the spontaneous emission of single nitrogen vacancy (NV) centers as their host diamond is reduced in size from a large monolithic crystal to a nanocrystal by successive cycles of oxidation. The size reduction induces a quenching of the NV radiative emission. Additional non-radiative channels lead to a decrease of the fluorescence intensity and the excited state lifetime. In one case, we observe the onset of blinking which may provide a route to understand these additional non-radiative decay channels.
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.