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IEEE Photonics Technology Letters

Enhanced Photoluminescence of Single-Photon Emitters in Nanodiamonds on a Gold Film

Yingzhi Chi, Gengxu Chen, Fedor Jelezko, E Wu, Heping Zeng

Published Jan 17, 2011• 35 citations
Publisher

Abstract

Engineering the photo-emission characteristics of single-photon emitters is crucial for the growing field of quantum technologies. We show that the photoluminescence of a single nitrogen-vacancy color center in nanodiamond could be significantly enhanced when attached to a gold film of 50 nm with preserving photophysical properties as a single photon source. The nitrogen-vacancy center on the gold film showed a decreased excited-state lifetime and a modified saturation characteristic. The photoluminescence enhancement was due to the enhanced electric field by the surface plasmon and the energy transfer from the excited state of nitrogen-vacancy centers to the surface plasmon.

DOI
10.1109/lpt.2011.2106488

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•Jan 1, 2014•0 citations
Engineering the photo-emission characteristics of single-photon emitters is crucial for the growing field of quantum technologies. We show that the photoluminescence of a single nitrogen-vacancy color center in nanodiamond could be significantly enhanced when attached to a gold film of 50 nm with preserving photophysical properties as a single photon source. The nitrogen-vacancy center on the gold film showed a decreased excited-state lifetime and a modified saturation characteristic. The photoluminescence enhancement was due to the enhanced electric field by the surface plasmon and the energy transfer from the excited state of nitrogen-vacancy centers to the surface plasmon.
We measured the second-order correlation function of the cathodoluminescence intensity and investigated the Purcell effect by comparing the lifetimes of quantum emitters with and without metal structure. The increase in the electromagnetic local density of state due to the coupling of a quantum emitter with a plasmonic structure causes a shortening of the emitter lifetime. Since the plasmon-enhanced electric field is confined well below the wavelength of light, the quantum emitter lifetime is changed in the nanoscale range. In this study, we combined cathodoluminescence in scanning (transmission) electron microscopy with Hanbury Brown--Twiss interferometry to measure the Purcell effect with nanometer and nanosecond resolutions. We used nitrogen-vacancy centers contained in nanodiamonds as the emitters and compared their lifetime in different environments: on a thin SiO2\mathrm{Si}{\mathrm{O}}_{2}SiO2​ membrane, on a thick flat silver film, and embedded in a silver film. The lifetime reductions of nitrogen-vacancy centers were observed in the samples with silver. We evaluated the lifetime by analytical calculation and numerical simulations and revealed the Purcell effects of emitters coupled to the propagating and localized surface plasmons.
Ultrafast emission rates obtained from quantum emitters coupled to plasmonic nanoantennas have recently opened fundamentally new possibilities in quantum information and sensing applications. Plasmonic nanoantennas greatly improve the brightness of quantum emitters by dramatically shortening their fluorescence lifetimes. Gap plasmonic nanocavities that support strongly confined modes are of particular interest for such applications. We demonstrate single-photon emission from nitrogen-vacancy (NV) centers in nanodiamonds coupled to nanosized gap plasmonic cavities with internal mode volumes about 10 000 times smaller than the cubic vacuum wavelength. The resulting structures features sub-nanosecond NV excited-state lifetimes and detected photon rates up to 50 million counts per second. Analysis of the fluorescence saturation allows the extraction of the multi-order excitation rate enhancement provided by the nanoantenna. Efficiency analysis shows that the NV center is producing up to 0.25 billion photons per second in the far-field.
Quantitative and reproducible optical characterization of single quantum emitters is crucial for quantum photonic materials research, yet accounting for measurement conditions remains challenging due to a lack of an established reference standard. We propose nanodiamonds containing single nitrogen vacancy (NV ? ) color centers as reliable, stable, and robust reference sources of single-photon emission. We select 4 potential reference emitter candidates from a study of thousands of NV ? centers. Candidates were remeasured at a second laboratory, correlating optical pump power and NV ? center emission intensity at saturation in addition to corresponding g (2) (0) values. A reference nanodiamond is demonstrated to account for experimental conditions, with reproducible and reliable single-photon emission, as a model for a new, to our knowledge, single-photon emitter reference standard.
The negatively-charged nitrogen vacancy (NV(-)) center in diamond is of great interest for quantum information processing and quantum key distribution applications due to its highly desirable long coherence times at room temperature. One of the challenges for their use in these applications involves the requirement to further optimize the lifetime and emission properties of the centers. Our results demonstrate the reduction of the lifetime of NV(-) centers, and hence an increase in the emission rate, achieved by modifying the refractive index of the environment surrounding the nanodiamond (ND). By coating the NDs in a polymer film, experimental results and numerical calculations show an average of 63% reduction in the lifetime and an average enhancement in the emission rate by a factor of 1.6. This strategy is also applicable for emitters other than diamond color centers where the particle refractive index is greater than the refractive index of the surrounding media.
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.
We report on an efficient room-temperature source of single photons based on single nitrogen-vacancy centers in nanodiamonds (NDs) placing on a large-area plasmonic platform formed by crystalline gold flakes covered with a thin dielectric layer. Due to the strongly confined plasmonic fields in the thin dielectric layer, the NDs show a large enhancement in the fluorescence intensity without significant degradation in single photon purity. According to the deduced fluorescence lifetime from g(2) measurements, the Purcell factor is estimated to be ~1.4. The plasmonic platform is very ideal for large-area fluorescence enhancement without the needs of sophisticated nanopositioning schemes for locating NDs at local hot spots in conventional plasmonic nanostructures.