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arXiv:1305.6405 · Applied Physics Letters

Tracking emission rate dynamics of nitrogen vacancy centers in nanodiamonds

Faraz Ahmed Inam, Andrew Mark Edmonds, Michael J. Steel, Stefania Castelletto

Published Jun 24, 2013• 26 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1063/1.4812711

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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.
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.
Abstract The nitrogen-vacancy colour centre in diamond is emerging as one of the most important solid-state quantum systems. It has applications to fields including high-precision sensing, quantum computing, single photon communication, metrology, nanoscale magnetic imaging and biosensing. For all of these applications, a high quantum yield of emitted photons is desirable. However, diamond samples engineered to have high densities of nitrogen-vacancy centres show levels of brightness varying significantly within single batches, or even within the same sample. Here we show that nearby nitrogen impurities quench emission of nitrogen-vacancy centres via non-radiative transitions, resulting in a reduced fluorescence quantum yield. We monitored the emission properties of nitrogen-vacancy centre ensembles from synthetic diamond samples with different concentrations of nitrogen impurities. All samples were irradiated with high energy electrons to create high densities of nitrogen-vacancy centres relative to the concentration of nitrogen impurities. While at low nitrogen densities of 1.81 ppm we measured a lifetime of 13.9 ns, we observed a strong reduction in lifetime with increasing nitrogen density. We measure a lifetime as low as 4.4 ns at a nitrogen density of 380 ppm. The change in lifetime matches a reduction in relative fluorescence quantum yield from 77.4% to 32% with an increase in nitrogen density from 88 ppm to 380 ppm, respectively. These results will inform the conditions required to optimise the properties of diamond crystals devices based on the fluorescence of nitrogen-vacancy centres. Furthermore, this work provides insights into the origin of inhomogeneities observed in high-density nitrogen-vacancy ensembles within diamonds and nanodiamonds.