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The Journal of Chemical Physics

Isolating and enhancing single-photon emitters for 1550 nm quantum light sources using double nanohole optical tweezers

Zohreh Sharifi, Michael Dobinson, Ghazal Hajisalem, Mirali Seyed Shariatdoust, Adriaan L. Frencken, Frank C. J. M. van Veggel, Reuven Gordon

Published May 14, 2021• 19 citations
Publisher

Abstract

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.

DOI
10.1063/5.0048728

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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 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 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.
In this thesis, an approach for developing single-photon sources at the 1550nm wavelength will be demonstrated, based on optical trapping of luminescent upconverting nanoparticles. A single-photon source is a source that emits a single photon at a time, and hence it is a source of quantum bits that constitutes the basic building units in quantum computers and quantum communications. The approach exploits the plasmonic properties of gold films and the waveguiding characteristics of single mode optical fibers (SMFs). We start by planar nanofabrication of subwavelength nanoapertures in a thin gold film based on finite difference time domain simulations for a peak transmission at the wavelength in question. Subsequently, using ultraviolet curable epoxy adhesion material, a nanoaperture patterned on a gold film can be transferred to an SMF tip forming a nanoantenna enhanced optical fiber tweezer (NAFT). As a final step in building the optical tweezer, a test of the capability of the integrated optical fiber tweezer to trap 20 nm, and 30nm polystyrene nanospheres, as well as luminescent upconverting nanoparticles (UCNPs), has been experimentally realized with encouraging results. In addition to the optical trapping of the luminescent nanoparticles, the nano aperture antenna can improve light coupling into the low loss optical fiber guiding channel. Also, it could have a positive influence on enhancing the photon emission rate through the Purcell effect. Furthermore, we have combined NAFT with a low insertion loss wave splitter, a wavelength-division multiplexer (WDM), to allow measuring the 1550nm photon-emission statistics on a cooled superconducting nanowire single-photon detector (SNSPD) at ~ 2.4o K. Eventually, nanoantenna enhanced optical fiber tweezers can play an essential role in optical trapping towards developing single-photon sources and the emerging technology of quantum information processing, computation, and cryptography.
Quantum light and in particular single photons have become essential resources for a growing number of quantum applications including quantum computing, quantum key distribution and quantum metrology. Solid-state atomlike systems such as semiconductor quantum dots and color defects in crystals have become the hallmark of highly pure single photon emitters in the past two decades. A particular interest has been developed in nanocrystal quantum dots (NQDs) and color centers in diamond as potential compact room-temperature emitters. There are however several challenges that inhibit the use of such sources in current technologies including low photon extraction efficiency, low emission rates and relatively low single photon purities. In this work we will review our efforts in overcoming these technical difficulties using several complementary methods including designing several nanoantenna devices that enhance the directionality and emission rate of the nanoemitter. In addition, we developed several temporal heralding techniques to overcome the hurdle of low single photon purity in NQDs in an effort to produce a highly pure, bright and efficient single photon source on-chip.
Conventional approaches to light-matter interactions rely on engineering photonic density of states. More recently, tailoring the spatial geometry of atoms or emitters themselves has emerged as a powerful and complementary route to control collective radiative properties. Here we experimentally realize a geometry-engineered ensemble of rare-earth ions by fabricating a periodic array of subwavelength gold nanoholes on lithium niobate implanted with thulium ions, forming a semi-two-dimensional array of quantum emitters embedded in a high-index crystalline thin film. The hybrid structure can simultaneously support localized and lattice plasmon resonances from the metallic array and collective atomic resonances from the ion ensemble. Using time-resolved photoluminescence and temperature-dependent measurements, we observe enhanced radiative emission attributed to collective atomic effects mediated by the nanohole lattice, distinct from single-emitter Purcell enhancement. Our results demonstrate a new regime of light-matter interaction opening a pathway toward broadband and scalable, geometry-controlled quantum optical interfaces in solid-state platforms.