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Nano Letters

Isolating Nanocrystals with an Individual Erbium Emitter: A Route to a Stable Single-Photon Source at 1550 nm Wavelength

Amirhossein Alizadehkhaledi, Adriaan L. Frencken, Frank C. J. M. van Veggel, Reuven Gordon

Published Dec 31, 2019• 37 citations
Publisher

Abstract

Single-photon emitters based on individual atoms or individual atomic-like defects are highly sought-after components for future quantum technologies. A key challenge in this field is how to isolate just one such emitter; the best approaches still have an active emitter yield of only 50% so that deterministic integration of single active emitters is not yet possible. Here, we demonstrate the ability to isolate individual erbium emitters embedded in 20 nm nanocrystals of NaYF 4 using plasmonic aperture optical tweezers. The optical tweezers capture the nanocrystal, whereas the plasmonic aperture enhances the emission of the Er and allows the measurement of discrete emission rate values corresponding to different numbers of erbium ions. Three separate synthesis runs show near-Poissonian distribution in the discrete levels of emission yield that correspond to the expected ion concentrations, indicating that the yield of active emitters is approximately 80%. Fortunately, the trap allows for selecting the nanocrystals with only a single emitter, and so this gives a route to isolating and integrating single emitters in a deterministic way. This demonstration is a promising step toward single-photon quantum information technologies that utilize single ions in a solid-state medium, particularly because Er emits in the low-loss fiber-optic 1550 nm telecom band.

DOI
10.1021/acs.nanolett.9b04165

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Single-photon emitters based on individual atoms or individual atomic-like defects are highly sought-after components for future quantum technologies. A key challenge in this field is how to isolate just one such emitter; the best approaches still have an active emitter yield of only 50% so that deterministic integration of single active emitters is not yet possible. Here, we demonstrate the ability to isolate individual erbium emitters embedded in 20 nm nanocrystals of NaYF 4 using plasmonic aperture optical tweezers. The optical tweezers capture the nanocrystal, whereas the plasmonic aperture enhances the emission of the Er and allows the measurement of discrete emission rate values corresponding to different numbers of erbium ions. Three separate synthesis runs show near-Poissonian distribution in the discrete levels of emission yield that correspond to the expected ion concentrations, indicating that the yield of active emitters is approximately 80%. Fortunately, the trap allows for selecting the nanocrystals with only a single emitter, and so this gives a route to isolating and integrating single emitters in a deterministic way. This demonstration is a promising step toward single-photon quantum information technologies that utilize single ions in a solid-state medium, particularly because Er emits in the low-loss fiber-optic 1550 nm telecom band.
Single-photon sources are required for quantum technologies and can be created from individual atoms and atom-like defects. Erbium ions produce single photons at low-loss fiber optic wavelengths, but they have low emission rates, making them challenging to isolate reliably. Here, we tune the size of gold double nanoholes (DNHs) to enhance the emission of single erbium emitters, achieving 50× enhancement over rectangular apertures previously demonstrated. This produces enough enhancement to show emission from single nanocrystals at wavelengths not seen in our previous work, i.e., 400 and 1550 nm. We observe discrete levels of emission for nanocrystals with low numbers of emitters and demonstrate isolating single emitters. We describe how the trapping time is proportional to the enhancement factor for a given DNH structure, giving us an independent way to measure the enhancement. This shows a promising path to achieving single emitter sources at 1550 nm.
Quantum technologies require sources of single photons, which can be created by isolating individual atoms or ions. Erbium ions are a promising choice for single photon sources as it emits photons at low-loss fiber optic wavelengths. However, erbium has a low emission rate and it is challenging to isolate single emitters reliably. Here, we isolate singly Er3+-doped nanocrystals using optical tweezers in a gold double nanohole aperture. The double nanohole geometry enhances the emission rate from the nanocrystals. With this additional enhancement we observe emission at 1550 nm. Discrete levels of emission from dilutely Er3+-doped nanocrystals are observed—corresponding to the number of active erbium emitters present. Nanocrystals with single active emitters were identified and isolated with this technique, demonstrating a path towards single emitter sources at 1550 nm.
Single photon sources are desired for quantum computing and communication applications. Ideally, these sources would provide single photons on demand at the low-loss fiber optical communication wavelength of 1550 nm. Single Erbium ions provide a good candidate for such sources because they emit at the right wavelength and they are very stable, however, the challenges remain of isolating a single emitter, coupling its emission to optical fiber and enhancing its emission rate. Nanoaperture optical tweezers provide a pathway to solving these issues by trapping and identifying single emitters, enhancing their emission rate and providing efficient coupling to an optical fiber. Recently, we have made progress in each of these areas (trapping, enhancing and coupling), which will be reviewed in this talk.
Achieving long lived (μs-scale) quantum coherence at room temperature in the telecom C band remains a central unsolved challenge for solid state quantum platforms, with coherence at this timescale previously demonstrated only under vacuum cryogenic conditions at temperatures over 600 times lower. To this end, we introduce a CMOS-compatible nanoengineering approach that deterministically controls the number of Er ions within a nanoscale volume and their electromagnetic environment using sub 5 nm silicon based hollow nanopillars, which achieves the first deterministic spatial isolation of single erbium ions. This nanostructure-enabled isolation suppresses ion-ion interactions and local electromagnetic field noise, enabling single-erbium-ion operation under ambient conditions. The resulting individually addressable single-ion devices exhibit record room temperature optical coherence times of T2* = ~32 μs in the telecom C-band (limited by the coherence of the laser) and extending to > 100 μs based on photon echo measurements. We further present the first demonstration of background free, upconversion enabled single photon emission from multilevel erbium qudits, providing high contrast coherent optical readout. Beyond these performance gains, our work, through sub-5-nm nanoscale engineering, establishes isolated single-ion environments as a viable route to room-temperature operation for solid-state quantum systems. This approach has the potential to address the long-standing barrier of room-temperature decoherence and open a manufacturable, telecom-compatible pathway toward scalable quantum networks, distributed sensing, and cryogenic-free quantum photonic integrated circuits.
Single atoms and atomlike defects in solids are ideal quantum light sources and memories for quantum networks. However, most atomic transitions are in the ultraviolet-visible portion of the electromagnetic spectrum, where propagation losses in optical fibers are prohibitively large. Here, we observe for the first time the emission of single photons from a single Er^{3+} ion in a solid-state host, whose optical transition at 1.5 μm is in the telecom band, allowing for low-loss propagation in optical fiber. This is enabled by integrating Er^{3+} ions with silicon nanophotonic structures, which results in an enhancement of the photon emission rate by a factor of more than 650. Dozens of distinct ions can be addressed in a single device, and the splitting of the lines in a magnetic field confirms that the optical transitions are coupled to the electronic spin of the Er^{3+} ions. These results are a significant step towards long-distance quantum networks and deterministic quantum logic for photons based on a scalable silicon nanophotonics architecture.
Single quantum emitters embedded in solid-state hosts are an ideal platform for realizing quantum information processors and quantum network nodes. Among the currently investigated candidates, Er^{3+} ions are particularly appealing due to their 1.5 μm optical transition in the telecom band as well as their long spin coherence times. However, the long lifetimes of the excited state-generally in excess of 1 ms-along with the inhomogeneous broadening of the optical transition result in significant challenges. Photon emission rates are prohibitively small, and different emitters generally create photons with distinct spectra, thereby preventing multiphoton interference-a requirement for building large-scale, multinode quantum networks. Here we solve this challenge by demonstrating for the first time linear Stark tuning of the emission frequency of a single Er^{3+} ion. Our ions are embedded in a lithium niobate crystal and couple evanescently to a silicon nanophotonic crystal cavity that provides a strong increase of the measured decay rate. By applying an electric field along the crystal c axis, we achieve a Stark tuning greater than the ion's linewidth without changing the single-photon emission statistics of the ion. These results are a key step towards rare earth ion-based quantum networks.