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Quantum 2.0 Conference and Exhibition

Optical and Spin Coherence Properties of Single Erbium Ions in Solid-State Hosts

Łukasz Dusanowski, Salim Ourari, Sebastian P. Horvath, Mehmet T. Uysal, Christopher M. Phenicie, Isaiah Gray, Mouktik Raha, S. Chen, Nathalie P. de Leon, Jeff D. Thompson

Published Jan 1, 2022• 0 citations
Publisher

Abstract

We study coherence of Er3+ ions implanted into solid-state hosts. Using heterogeneously integrated photonic crystal cavities, we isolate single ions, and probe their optical and spin properties using resonance fluorescence and optically detected magnetic resonance.
DOI
10.1364/quantum.2022.qth2b.2

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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.

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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.
Light-matter interaction at single quantum object level is a long-lived challenge and dream of physicists. From the 1970s, the development of single ion spectroscopy and the observation of single photon states pave a way to a new era of detecting, and coherently manipulating quantum objects with electromagnetic field at single-ion levels. Later on, the invention of single molecular spectroscopy offers a new approach to investigate single quantum objects in condensed matter, where the sophisticated trapping systems like in ions and cold atoms are not needed, resulting in the discovery of various of single photon emitters embedded in solids. Among all, single quantum dots and single negatively charged nitrogen-vacancy centers in diamond attract most attentions, since their single spins can be coherently manipulated and entangled by the light field giving rise to numerous applications from nanoscale sensing to quantum computing. They are intensively studied as the most promising candidates for the realization of solid-state quantum bits. However, these systems coupled to a complex environment which can result in rapid loss of spin coherence or optical instability. Finding an alternative solid-state single system with remarkable optical and spin properties is the motivation of this dissertation. Rare earth ions doped in inorganic crystal hosts provide promises not only by the high quality factor 4f-4f optical transitions but also by the well preserved and long-lived spin states, with the applications from solid-state laser spectroscopy to quantum information processing. However, for almost three decades, not being able to identify single rare earth elements in solids is the obstacle to achieve their full potential functionality. We demonstrated the first direct optical detection of single rare earth ions (praseodymium) in solids in 2012. This research was covered in my Master Degree Thesis. This dissertation presents experimental progress in optically detecting other single rare earth species in crystals, understanding their fundamental spectroscopy properties and coherently controlling them, which is mainly focused on single trivalent cerium ions in different host materials. Following the optical detection of single cerium ions in yttrium aluminum garnet (YAG), the optical and spin properties of single Ce ions are investigated. Single Ce ions show good photostability under the pulsed laser excitation. Still, like in other solid emitters, photo-induced dynamics of single Ce ions is observed, however, in a counterintuitive way under the continuous laser irradiation. To understand this behavior, we proposed a charge dynamics model, and developed a novel method to suppress this undesired charge dynamics. With this approach, we obtain the photoluminescence excitation spectrum of single Ce ions in YAG under a CW laser excitation. Narrow (~80 MHz) and spectrally stable optical transitions between the lowest Kramers doublets of the ground and the excited states are observed. In comparison with the large inhomogeneous broadening (500 GHz), narrow resonant transitions provide the good selectivity in the spectral domain. Moreover, the single Ce ground spin state presents a spin 1/2 system with anisotropy g factor. It results in the optical selection rules dependent on the directions of the external magnetic field. Under parallel external magnetic field with respect to the quantization axis, only the spin-flip transitions are allowed with high transition contrast. It gives the opportunity to optically initialize the ground spin state of single Ce ions with 97.5% fidelity. The coherent spin properties of single Ce ions can be investigated, after the successful optical initialization. By scanning the microwave frequency, we obtain the electron spin resonance of single Ce spin transitions. We show the spin state has a coherence time of 290 ns, which is dominated by the surrounding aluminum nuclear spin bath and impurities induced electron spin bath. The coherence time can be extended to 2 ms through dynamical decoupling method, which approaches closely to the upper limit 4.5 ms due to spin-lattice relaxation. This result indicates single Ce electron spin can be a good solid-state qubit. With the combination of optical and spin manipulations of single Ce ions, a quantum interface between a single spin and a single photon is observed by monitoring the temporal behavior of circularly polarized emission photons from the ion. We obtain the Larmor precession of the excited spin state, indicating the direct mapping of the excited spin states of single Ce ions onto the polarization states of the fluorescence photons. Furthermore, with both optical and spin access, we all-optically demonstrate coherent population trapping of a single Ce spin qubit. To scale up the system for further applications, we present the nano-scale engineering of rare earth species in YAG crystal, with the acquirement of the production yield of Ce and Pr implantation (53 and 91% respectively). The optical and spin properties of single implanted Ce ions show fairly good performance, which paves the way towards coherent coupling of single rare earth qubits in a small volume. Besides the study of single Ce ions, the spectroscopy properties of single praseodymium ions in YAG crystal are investigated. We obtain the photoluminescence excitation spectrum and the hyperfine splitting of a single praseodymium ion. All-optical control of a single praseodymium ion is achieved. In this dissertation, we solve the key problem of optically detecting, spectrally studying and coherently manipulating single rare earth ions in solids. The developed methods including optical detection, initialization, readout, coherent control and nanoscale production of single rare earth elements in crystals offer novel and powerful tools for understanding and exploring the fundamental spectroscopy properties of single rare earth elements in solids. It paves a way towards constructing scalable quantum network based on single rare earth solid-state qubits.
Entanglement between single spins and photons is an important resource in quantum information science, e.g. in quantum networking. Rare-earth ions in dielectric crystals have emerged as a promising candidate for this task. Rare-earth ion doped solids have been used so far mostly as ensemble-based quantum memories. However, they also feature promising properties for single ion detection and manipulation, such as long-lived spins, narrow optical transitions and preservation of coherence properties when inserted in nanostructures. Because of the long lifetimes of the optical t
As an active material with favorable linear and nonlinear optical properties, thin-film lithium niobate has demonstrated its potential in integrated photonics. Integration with rare-earth ions, which are promising candidates for quantum memories and transducers, will enrich the system with new applications in quantum information processing. Here, we investigate the optical properties at 1.5 μm wavelengths of rare-earth ions (Er3+) implanted in thin-film lithium niobate waveguides and micro-ring resonators. Optical quality factors near a million after post-annealing show that ion implantation damage can be repaired. The transition linewidth and fluorescence lifetime of erbium ions are characterized. The ion-cavity coupling is observed through a Purcell enhanced fluorescence from which a Purcell factor of 3.8 ± 0.5, compared with waveguide lifetime, is extracted. This platform is compatible with top-down lithography processes and leads to a scalable path for controlling spin-photon interfaces in photonic circuits.