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arXiv:2012.11224 · Physical review. B./Physical review. B

Purcell effect of nitrogen-vacancy centers in nanodiamond coupled to propagating and localized surface plasmons revealed by photon-correlation cathodoluminescence

Sotatsu Yanagimoto, Naoki Yamamoto, Takumi Sannomiya, K. Akiba

Published May 14, 2021• 31 citations

Abstract

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 $\mathrm{Si}{\mathrm{O}}_{2}$ 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.

DOI: 10.1103/physrevb.103.205418

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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

\mathrm{Si}{\mathrm{O}}_{2}

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.

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.

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.

Spontaneous emission (SE) of nitrogen-vacancy centers (NV-centers), which are contained in a single nanodiamond (ND), placed near a silver nanocube, is investigated both experimentally and theoretically. The ND-cube system is assembled with an atomic force microscope, allowing us to directly compare its SE properties to that of the isolated ND. It is demonstrated that the cube coupled NV-centers exhibit strongly polarized SE. For optimal pump laser polarization, the rate of photons is enhanced by a factor of 4.1, with the excited state lifetime being reduced by a factor of 4.1. The enhancement of photon rate is a consequence of local field enhancement of the pump laser, while the SE polarization and lifetime reduction results from coupling of NV-centers to the localized surface plasmon mode of the nanocube. The experimental observations are in qualitative agreement with the model of SE from randomly oriented electric dipoles, allowing us to reveal the underlying physics of the investigated configuration.

Precise detection of surface plasmons is crucial for the research of nanophotonics and quantum optics. In this Letter, we used a single nitrogen vacancy center in diamond as a probe to detect the surface plasmon that was tuned by the thickness of a metallic film. The fluorescence intensity and lifetime of the nitrogen vacancy (NV) center were measured to obtain the information of local light-matter interaction. A nonlinear thickness dependent change of the surface plasmon was observed, with the maximum at the thickness of approximately 30 nm. With optimized thickness of silver film, the fluorescence intensity of a single NV center was enhanced 2.6 times, and the lifetime was reduced by a factor of 3, without affecting the coherence time of the NV spin state. The results proved that this system can quantitatively detect the light-matter interaction at nanoscale, and it provides an approach to enhance the fluorescence intensity of a quantum emitter.

Solid-state quantum emitters are in high demand for emerging technologies such as advanced sensing and quantum information processing. Generally, these emitters are not sufficiently bright for practical applications, and a promising solution consists in coupling them to plasmonic nanostructures. Plasmonic nanostructures support broadband modes, making it possible to speed up the fluorescence emission in room-temperature emitters by several orders of magnitude. However, one has not yet achieved such a fluorescence lifetime shortening without a substantial loss in emission efficiency, largely because of strong absorption in metals and emitter bleaching. Here, we demonstrate ultrabright single-photon emission from photostable nitrogen-vacancy (NV) centers in nanodiamonds coupled to plasmonic nanocavities made of low-loss single-crystalline silver. We observe a 70-fold difference between the average fluorescence lifetimes and a 90-fold increase in the average detected saturated intensity. The nanocavity-coupled NVs produce up to 35 million photon counts per second, several times more than the previously reported rates from room-temperature quantum emitters.