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Applied Physics Letters

Enhancing erbium optical emission rate via high-throughput host crystal selection

Gregory D. Grant, Swarnabha Chattaraj, Chelsie Hadley, F. Joseph Heremans, D. D. Awschalom, Jiefei Zhang, Giulia Galli, Supratik Guha

Published Sep 7, 2026• 0 citations
Publisher

Abstract

Erbium-doped solid-state crystals present an attractive platform for quantum communication, combining the telecom C-band spin–photon interface and long coherence times of erbium (Er3+) with the versatility of solid-state hosts. However, across commonly investigated materials, Er3+ is a “dim” ion, with low optical emission rates of kilohertz at most. This makes implementing quantum information transfer protocols (e.g., quantum teleportation) at usable rates a major challenge. One route to increasing Er3+ radiative rates is by careful selection of crystal hosts: the crystal field around an Er3+ ion may hybridize states of different parity, potentially increasing the radiative rate of its telecom transition. Here, using high-throughput computational methods, the radiative rates of Er3+ embedded in 9215 materials are estimated. The computation shows that careful host selection could increase Er3+ radiative rates by an order of magnitude compared to commonly studied hosts. Calculated results are compared with experimental radiative rates in a subset of materials, finding notable clustering but weak correlation. Nevertheless, the “brightest” candidates combined with suitable nanophotonics engineering could push Er3+-based quantum memories into the megahertz bandwidth regime.

DOI
10.1063/5.0328217

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Applied Physics Letters•Sep 18, 2023•4 citations
Erbium-doped solid-state crystals present an attractive platform for quantum communication, combining the telecom C-band spin–photon interface and long coherence times of erbium (Er3+) with the versatility of solid-state hosts. However, across commonly investigated materials, Er3+ is a “dim” ion, with low optical emission rates of kilohertz at most. This makes implementing quantum information transfer protocols (e.g., quantum teleportation) at usable rates a major challenge. One route to increasing Er3+ radiative rates is by careful selection of crystal hosts: the crystal field around an Er3+ ion may hybridize states of different parity, potentially increasing the radiative rate of its telecom transition. Here, using high-throughput computational methods, the radiative rates of Er3+ embedded in 9215 materials are estimated. The computation shows that careful host selection could increase Er3+ radiative rates by an order of magnitude compared to commonly studied hosts. Calculated results are compared with experimental radiative rates in a subset of materials, finding notable clustering but weak correlation. Nevertheless, the “brightest” candidates combined with suitable nanophotonics engineering could push Er3+-based quantum memories into the megahertz bandwidth regime.
Abstract Doping erbium ions into europium-based hosts offers a promising platform for quantum repeater nodes, combining europium’s exceptional coherence properties for long-term quantum storage with erbium’s microwave compatibility and direct telecom-band emission for efficient optical interfacing. In this work, we investigated erbium-doped EuCl3 · 6H2O stoichiometric crystals as a candidate for such nodes. We demonstrate that erbium doping shifts the optical transition frequencies of nearby Eu3+ ions, producing well resolved satellite lines in the inhomogeneous absorption profile. We experimentally probe the coupling between Er3+ and Eu3+ ions under varying temperature and magnetic field conditions, quantifying the interaction strength, which ranges from tens to hundreds of kilohertz, depending on field orientation, magnitude, and the lattice position of the Eu3+ ions. At 60 mK and a moderate magnetic field of 0.1 T, we observed a strong frozen core effect from Er3+ spins, substantially extending the Eu3+ optical coherence time from 62 us to 162 us, approaching the lifetime limit, and enabling hour-long hyperfine state lifetimes. These results underscore the potential of dual-species rare-earth systems for photonic quantum technologies and highlight their promise for precise quantum control.
Rare-earth ions in solid-state hosts are a compelling hardware platform for quantum networking due to their exceptional optical, and long-lived spin transitions. Erbium's transitions couple to photons in the Telecom-C band, making it compatible with fibre, and has demonstrated high coherence and low spectral diffusion in a range of materials. However, it has a low optical dipole moment, leading to low light-matter coupling. This limits the rate at which operations performed within a network. Despite decades of research, Er transitions remain poorly understood. Hosts are chosen based on convention, convenience, and (well-informed) heuristics, since calculations of the properties of lanthanide 4f shell are prohibitively difficult. This thesis addresses the challenge of this weak dipole through two complementary approaches; both of which constitute engineering the erbium-crystal system. Firstly, we engineer the emitter itself, from the bottom up. We seek an optimal crystal site for ions, which maintains coherence but increases transition strength. To this end, we have characterised four Er sites in CaF2 to understand how the crystal field affects ion properties. We identify sites with dipole moments as high as 1.63x10^-32 Cm despite lifetimes in excess of 10 ms, and coherence of up to 43.9 µs. This informs our next steps, in selecting an optimal site for single ion addressing, and our long-term goal of designing sites for high dipole moments. In the second approach, we engineer the crystal from the top down, fabricating whispering gallery mode resonators in calcium fluoride. I have fabricated five high Q resonators in doped and undoped CaF2, and commenced their characterisation. We have prototyped a coupler for use of these devices in a cryostat with no free-space optical access. This engineered crystal system - a high dipole erbium site coupled to a high Q resonator - provides a path toward competitive optical cooperativity for single erbium ions in the solid state.
The implementation of scalable quantum networks requires photons at the telecom band and long-lived spin coherence. The single Er3+ in solid-state hosts is an important candidate that fulfills these critical requirements simultaneously. However, to entangle distant Er3+ ions through photonic connections, the emission frequency of individual Er3+ in solid-state matrix must be the same, which is challenging because the emission frequency of Er3+ depends on its local environment. Herein, we propose and experimentally demonstrate the Stark tuning of the emission frequency of a single Er3+ in a Y2SiO5 crystal by employing electrodes interfaced with a silicon photonic crystal cavity. We obtain a Stark shift of 182.9±0.8 MHz, which is approximately 27 times of the optical emission linewidth, demonstrating promising applications in tuning the emission frequency of independent Er3+ into the same spectral channels. Our results provide a useful solution for construction of scalable quantum networks based on single Er3+ and a universal tool for tuning emission of individual rare-earth ions.
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.
Abstract Erbium ion is among the most promising solid-state single photon emitters and spin-photon interfaces for quantum networks, emitting directly in the telecom C-band in many host semiconductors. Recently, the search for scalable, low-noise host materials turned toward atomically thin and van der Waals materials that enable efficient integration with nanopho-tonic architectures. Here, we identify talc, a naturally occurring layered magnesium silicate, as a promising host for telecom-active erbium centers. Using first-principles density functional theory combined with multireference wavefunction calculations, we investigate the thermodynamic stability, electronic structure, crystal-field splitting, and optical transitions of erbium-related defects in talc. We find that substitutional incorporation of Er at Mg sites is energetically favourable over a wide range of Fermi-levels, leading predominantly to telecom C band emitting Er3+ configuration. The characteristic 4I13/2 → 4I15/2 transition of Er3+ is preserved in the talc environment and remains centred near 1.55 µm, while crystal-field interactions produce a Stark manifold suitable for spectrally selective optical addressing. The combination of thermodynamic stability, wide band gap, low background emission, and compatibility with van der Waals heterostructures suggests that erbium-doped talc constitutes a 1 promising platform for integrated photonics in the C-band.
Atomic-like emitters in the solid state serve as important resources in the advancement of future quantum networks. In particular, intra-4f optical transitions of rare earth ions exhibit excellent coherence properties thanks to the shielding effect of outer electrons. Still, the presence of various dephasing channels in solid state hosts introduces additional decoherence beyond the radiative decay, causing the coherence time of most rare earth doped materials to be over an order of magnitude lower than the radiative limit. Such obstacle prevents the emission of indistinguishable photons from rare earth ions, which is an essential requirement for various quantum applications. In this work, we perform optical coherence study on erbium ions doped in thin-film lithium niobate by patterning photonic crystal resonators with quality factor around 100 k and sub-λ3 mode volume. Leveraging the combination of long coherence and strong Purcell enhancement in the cavity, we show that the coherence time measured with photon echo approaches the radiative limit (80%), representing a 50-fold improvement compared to the waveguide case. Our results present promising prospects toward utilizing rare earth doped materials as quantum repeaters and sources of indistinguishable photons.