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arXiv:1001.3882 · Optics Express

Spontaneous emission of a nanoscopic emitter in a strongly scattering disordered medium

Paul V. Ruijgrok, R. Wüest, Aleksander A. Rebane, Alois Renn, Vahid Sandoghdar

Published Mar 12, 2010• 46 citations
arXivHTMLPDF

Abstract

Fluorescence lifetimes of nitrogen-vacancy color centers in individual diamond nanocrystals were measured at the interface between a glass substrate and a strongly scattering medium. Comparison of the results with values recorded from the same nanocrystals at the glass-air interface revealed fluctuations of fluorescence lifetimes in the scattering medium. After discussing a range of possible systematic effects, we attribute the observed lengthening of the lifetimes to the reduction of the local density of states. Our approach is very promising for exploring the strong threedimensional localization of light directly on the microscopic scale.

DOI
10.1364/oe.18.006360

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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Mar 28, 2013•0 citations
Fluorescence lifetimes of nitrogen-vacancy color centers in individual diamond nanocrystals were measured at the interface between a glass substrate and a strongly scattering medium. Comparison of the results with values recorded from the same nanocrystals at the glass-air interface revealed fluctuations of fluorescence lifetimes in the scattering medium. After discussing a range of possible systematic effects, we attribute the observed lengthening of the lifetimes to the reduction of the local density of states. Our approach is very promising for exploring the strong threedimensional localization of light directly on the microscopic scale.
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.
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.
Summary form only given. Over more than three decades many experiments have shown that the rate of spontaneous emission from an emitter can be strongly modified due to its electromagnetic surrounding. It is also well-known that the fluorescence lifetime of an emitter changes when embedded in dielectric media where aside from a change in the density of states, it is influenced by the local fields in the dielectric. The goal of our work has been to study the transition between the regime of an emitter in vacuum to that of a bulk dielectric medium, emphasizing the domain where the emitter's environment has a subwavelength extent. In our experiment we have investigated the dependence of the spontaneous emission rate of Eu/sup 3+/ ions in polymer nanospheres of different diameters, ranging from 20nm to 2000nm. In order to perform well-defined control experiments, we have combined atomic force microscopy and fluorescence confocal microscopy to make measurements only on isolated single spheres lying on a glass substrate.
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.