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Nano Letters

Ultrabright Room-Temperature Sub-Nanosecond Emission from Single Nitrogen-Vacancy Centers Coupled to Nanopatch Antennas

Simeon Bogdanov, Mikhail Y. Shalaginov, Alexei Lagutchev, Chin‐Cheng Chiang, Deesha Shah, Alexandr S. Baburin, Ilya A. Ryzhikov, Ilya A. Rodionov, Alexander V. Kildishev, Alexandra E. Boltasseva, Vladimir M. Shalaev

Published Jul 3, 2018• 172 citations
Publisher

Abstract

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.

DOI
10.1021/acs.nanolett.8b01415

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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.
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.
Abstract Integrated on‐demand single‐photon sources are critical for the implementation of photonic quantum information processing systems. To enable practical quantum photonic devices, the emission rates of solid‐state quantum emitters need to be substantially enhanced and the emitted signal must be directly coupled to an on‐chip circuitry. The photon emission rate speed‐up is best achieved via coupling to plasmonic antennas, while on‐chip integration can be realized by directly coupling emitters to photonic waveguides. The realization of practical devices requires that both the emission speed‐up and efficient out‐coupling are achieved in a single architecture. Here, a novel architecture is proposed that combines chip compatibility with high radiative emission rates—a quantum plasmonic launcher. The proposed launchers contain single nitrogen‐vacancy (NV) centers in nanodiamonds as quantum emitters that offer record‐high average fluorescence lifetime shortening factors of about 7000 times. Nanodiamonds with single NVs are sandwiched between two silver films that couple more than half of the emission into in‐plane propagating surface plasmon polaritons. This simple, compact, and scalable architecture represents a crucial step toward the practical realization of high‐speed on‐chip quantum networks.
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.
We demonstrate an exceptionally bright photon source based on a single nitrogen-vacancy center (NV center) in a nanodiamond (ND) placed in the nanoscale gap between two monocrystalline silver cubes in a dimer configuration. The system is operated near saturation at a stable photon rate of 850 kcps, while we further achieve strongly polarized emission and high single photon purity, evident by the measured autocorrelation with a g (2) (0) value of 0.08. These photon source features are key parameters for quantum technological applications, such as secure communication based on quantum key distribution. The cube antenna is assembled with an atomic force microscope, which allows us to predetermine the dipole orientation of the NV center and optimize cube positioning accordingly, while also tracking the evolution of emission parameters from isolated ND to the one- and two-cube configuration. The experiment is well described by finite element modeling, assuming an instrinsic quantum efficiency of 0.35. We attribute the large photon rate of the assembled photon source, to increased quantum efficiency of the NV center and high antenna efficiency.
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.
Unlocking the quantum potential of nitrogen-vacancy (NV) centers in diamonds has led to innovative advancements in sensing applications. By coupling NV centers with plasmonic nanostructures, ultrasensitive biolabels are envisioned. To this end, we exploit DNA self-assembly to create hybrid plasmonic nanodiamonds, featuring a closed nanocavity encapsulating a single nanodiamond. Correlated spectroscopy reveals enhanced brightness and emission rates, crucial for quantum sensing. This synergy between plasmonics and diamond fluorescence augments photon emission intensity and accelerates emission rates, enabling improved temporal resolution. These nanodiamonds hold promise as stable single-photon sources and versatile platforms for probing quantum effects in biology. This talk highlights the development, properties, and potential applications of these nanodiamonds, bridging quantum sensing and biomedicine, and fostering transformative changes in biophotonics.