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Decay rate statistics of NV centres in diamond on plasmonic and dielectric substrates

Hao Li, Jun‐Yu Ou, Nikitas Papasimakis, V.A. Fedotov, Nikolay I. Zheludev

Published Sep 16, 2019• 0 citations
OpenAlex

Abstract

We study experimentally the statistics of the emission characteristics of NV0 centres in diamond nanoparticles in different dielectric environments. Diamond nanoparticleswith sizes of ~120 nm each containing a large number of NV centres (>1000) are deposited on different substrates, including dielectrics (silicon, silicon nitride, diamond) and plasmonic metals (silver). We record lifetime and emission spectra by time-resolved cathodoluminescence (TR-CL). For each different substrate we collect data from 60 different clusters of particles and study the statistics of their emission properties. We observe a strong variation of the lifetime statistics in different substrates, with the shortest average decay rate and narrowest distribution occurring in the case of diamond substrate. On the other hand, plasmonic (Ag) and high index dielectric (Si) substrate result in longer lifetimes and substantially broader distributions. Our results provide insights into the role of the dielectric environment and indicate the presence of complex interactions with the substrate.

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We study experimentally the statistics of the emission characteristics of NV0 centres in diamond nanoparticles in different dielectric environments. Diamond nanoparticleswith sizes of ~120 nm each containing a large number of NV centres (>1000) are deposited on different substrates, including dielectrics (silicon, silicon nitride, diamond) and plasmonic metals (silver). We record lifetime and emission spectra by time-resolved cathodoluminescence (TR-CL). For each different substrate we collect data from 60 different clusters of particles and study the statistics of their emission properties. We observe a strong variation of the lifetime statistics in different substrates, with the shortest average decay rate and narrowest distribution occurring in the case of diamond substrate. On the other hand, plasmonic (Ag) and high index dielectric (Si) substrate result in longer lifetimes and substantially broader distributions. Our results provide insights into the role of the dielectric environment and indicate the presence of complex interactions with the substrate.
We observe a strong variation of the lifetime statistics of nanodiamonds (NDs) in different substrates: NDs on silicon and silver exhibit longer lifetimes and broader distributions than NDs on silicon nitride and diamond film . On the other hand, the diamond substrate results in the shortest average decay rate and narrowest distribution. Our results provide insights into the role of the dielectric environment we argue that they indicate the presence of complex interactions with the substrate related to the difference in optical properties between the diamond nanoparticles in which the emitters are situated and the substrate.
We study the properties of luminescent diamond particles of different sizes (up to ~1.5 μ m) containing multiple NV-centers. We theoretically predict that the average liftetime in such particles is decreased by several times as compared to optically small subwavelength nanodiamonds. In our experiments, samples were obtained by milling the plasma-enhanced chemical vapor deposited diamond film, and characterized by Raman spectroscopy and dark- field spectroscopy methods. Time-resolved luminescence measurements of the excited state of NV-centers showed that their average lifetime varies from 10 to 17 ns in different samples. By comparing this data to the values of the lifetime of the NV-centers in optically small nanodiamonds, known from literature, we confirm a severalfold decrease of the lifetime in resonant particles.
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.
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.
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.