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arXiv:2103.08774 · Optics Express

Decay rate enhancement of diamond NV-centers on diamond thin films

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

Published Jun 24, 2021• 0 citations
arXivHTMLPDF

Abstract

We demonstrate experimentally two-fold enhancement of the decay rate of NV° centers on diamond/Si substrate as opposed to a bare Si substrate. We link the decay enhancement to the interplay between the excitation of substrate modes and the presence of non-radiative decay channels. We show that the radiative decay rate can vary by up to 90% depending on the thickness of the diamond film.

DOI
10.1364/oe.425706

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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Mar 28, 2013•0 citations
We demonstrate experimentally two-fold enhancement of the decay rate of NV° centers on diamond/Si substrate as opposed to a bare Si substrate. We link the decay enhancement to the interplay between the excitation of substrate modes and the presence of non-radiative decay channels. We show that the radiative decay rate can vary by up to 90% depending on the thickness of the diamond film.
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.
This thesis decay rate enhancement and photophysics of nitrogen vacancy (NV) centers in diamond and quantum emitters in hexagonal boron nitride (hBN). The NV center in diamond is a unique physical system that finds use in many quantum technologies such as quantum sensing, quantum information processing and single photon generation. Consisting of a substitutional nitrogen atom next to a vacant lattice site, the NV center introduces discrete electronic energy levels within the wide bandgap of diamond. The NV center can be optically excited and will emit single photons upon relaxation that hold information of the spin state of the NV center. In this thesis, we use metallic structures to modify and enhance the decay rate of NV centers in bulk and nano diamonds in three different experiments. Such an enhancement is a way to improve the usability of NV as a single photon source. Using TiN films with metamaterial properties we observe a 2-fold decrease of the total excited state lifetime of NV centers in nano diamonds, when comparing to similar NV centers not influenced by the TiN films. For shallow implanted NV centers in bulk diamond we experimentally investigate how a decay rate enhancement influences the signal-to-noise ratio (SNR) in spin readout measurements. In this experiment we perform spin state readout before and after introducing a rate enhancement and find a 30 % drop in spin contrast. We model the spin readout measurements using a five-level model and use that to predict the SNR under higher rate enhancement. In the last NV related experiment we use a curved metallic mirror on top of shallow implanted NV centers, to measure the continuous lifetime modification as a function of distances to the mirror. This allows us to determine the internal quantum efficiency (IQE) by fitting the experimental data with a model that includes calculating the expected Purcell factor. We find IQE values of 0.70±0.07 and 0.82±0.08 for implantation depths of 4.5±1 and 8±2 nm, respectively. Last but not least, newly discovered bright single photon emitters in two dimensional hBN were investigated. Similar to the NV center they are believed to be crystal defects, but the defect configuration is not fully known. In this thesis, the photophysics of quantum emitters in hBN nano flakes are investigated. Intensity autocorrelation measurements indicate the presence of at least two metastable states, seen by distinct photon bunching levels on long time scales in the g(2)(τ)-functions. We also observe blinking behaviour, which we show can be explained by changes in the IQE. From rate equation fitting we find that transition rates scale linearly with excitation power. Based on the transition rates we estimate the IQE to be close to unity for excitation powers below saturation.
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.
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.
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.