arXiv:2406.08167 · Materials for Quantum Technology
Optical investigations of coherence and relaxation dynamics of a thulium-doped yttrium gallium garnet crystal at sub-kelvin temperatures for optical quantum memory
Antariksha Das, Mohsen Falamarzi Askarani, Jacob H. Davidson, Neil E. Sinclair, Joshua A. Slater, Sara Marzban, Daniel Oblak, Charles W. Thiel, R. L. Cone, Wolfgang Tittel
Abstract Rare-earth ion-doped crystals are of great interest for quantum memories, a central component in future quantum repeaters. To assess the promise of 1 % Tm3+-doped yttrium gallium garnet (Tm:YGG), we report measurements of optical coherence and energy-level lifetimes of its 3H 6 ↔ 3 H4 transition at a temperature of around 500 mK and various magnetic fields. Using spectral hole burning (SHB), we find hyperfine ground-level (Zeeman level) lifetimes of several minutes at magnetic fields of less than 1000 G. We also measure coherence time exceeding one millisecond using two-pulse photon echoes. Three-pulse photon echo and SHB measurements reveal that due to spectral diffusion, the effective coherence time reduces to a few µs over a timescale of around two hundred seconds. Finally, temporal and frequency-multiplexed storage of optical pulses using the atomic frequency comb protocol is demonstrated. Our results suggest Tm:YGG to be promising for multiplexed photonic quantum memory for quantum repeaters.
Abstract Rare-earth ion-doped crystals are of great interest for quantum memories, a central component in future quantum repeaters. To assess the promise of 1 % Tm3+-doped yttrium gallium garnet (Tm:YGG), we report measurements of optical coherence and energy-level lifetimes of its 3H 6 ↔ 3 H4 transition at a temperature of around 500 mK and various magnetic fields. Using spectral hole burning (SHB), we find hyperfine ground-level (Zeeman level) lifetimes of several minutes at magnetic fields of less than 1000 G. We also measure coherence time exceeding one millisecond using two-pulse photon echoes. Three-pulse photon echo and SHB measurements reveal that due to spectral diffusion, the effective coherence time reduces to a few µs over a timescale of around two hundred seconds. Finally, temporal and frequency-multiplexed storage of optical pulses using the atomic frequency comb protocol is demonstrated. Our results suggest Tm:YGG to be promising for multiplexed photonic quantum memory for quantum repeaters.
Long optical storage times are an essential requirement to establish high-rate entanglement distribution over large distances using memory-based quantum repeaters. Rare earth ion-doped crystals are arguably well-suited candidates for building such quantum memories. Toward this end, we investigate the 795.32 nm 3H6 ↔ 3H4 transition of 1% thulium-doped yttrium gallium garnet crystal (Tm3+:Y3Ga5O12 : Tm3+:YGG). Most essentially, we find that the optical coherence time can reach 1.1 ms, and, using laser pulses, we demonstrate optical storage based on the atomic frequency comb (AFC) protocol up to 100 µs. In addition, we demonstrate multiplexed storage, including feed-forward selection, shifting, and filtering of spectral modes, as well as quantum state storage using members of non-classical photon pairs. Our results show that Tm:YGG can be a potential candidate for creating multiplexed quantum memories with long optical storage times.
Decoherence of the 795 nm 3H6 to 3H4 transition in 1 (Tm:YGG) is studied at temperatures as low as 1.2 K. The temperature, magnetic field, frequency, and time scale (spectral diffusion) dependence of the optical coherence lifetime is measured. Our results show that the coherence lifetime is impacted less by spectral diffusion than other known thulium-doped materials. Photon echo excitation and spectral hole burning methods reveal uniform decoherence properties and the possibility to produce full transparency for persistent spectral holes across the entire 56 GHz inhomogeneous bandwidth of the optical transition. Temperature-dependent decoherence is well described by elastic Raman scattering of phonons with an additional weaker component that may arise from a low density of glass-like dynamic disorder modes (two-level systems). Analysis of the observed behavior suggests that an optical coherence lifetime approaching 1 ms may be possible in this system at temperatures below 1 K for crystals grown with optimized properties. Overall, we find that Tm:YGG has superior decoherence properties compared to other Tm-doped crystals and is a promising candidate for applications that rely on long coherence lifetimes, such as optical quantum memories and photonic signal processing.
The magnetic properties of crystals doped with rare-earth ions have long been studied for their long coherence times and applications in signal processing. Here, the authors measure a complete tensor description of the hyperfine structure for a pair of optically addressable levels belonging to the Tm3+-ion defects within the host material. Certain orientations of interest stand out, such as some that realize optical clock transitions; they are shown to have an invariant response to fluctuations in the local magnetic environment.
We argue that long optical storage times are required to establish entanglement at high rates over large distances using memory-based quantum repeaters. Triggered by this conclusion, we investigate the 795.325nm3 ${\mathrm{H}}_{6}\ensuremath{\leftrightarrow}{^{3}\mathrm{H}}_{4}$ transition of Tm:Y3Ga5O12 (Tm:YGG). Most importantly, we find that the optical coherence time can reach 1.1 ms, and, using laser pulses, we demonstrate optical storage based on the atomic frequency comb protocol during up to $100\text{ }\text{ }\ensuremath{\mu}\mathrm{s}$ as well as a memory decay time Tm of $13.1\text{ }\text{ }\ensuremath{\mu}\mathrm{s}$. Possibilities of how to narrow the gap between the measured value of Tm and its maximum of $275\text{ }\text{ }\ensuremath{\mu}\mathrm{s}$ are discussed. In addition, we demonstrate multiplexed storage, including with feed-forward selection, shifting and filtering of spectral modes, as well as quantum state storage using members of nonclassical photon pairs. Our results show the potential of Tm:YGG for creating multiplexed quantum memories with long optical storage times, and open the path to repeater-based quantum networks with high entanglement distribution rates.
Abstract We report a detailed investigation of spin relaxation dynamics in the rare-earth-doped crystal 171 Yb:Y 2 SiO 5 , a promising platform for quantum memory based on atomic frequency combs. The population dynamics among the four ground-state hyperfine levels were studied in the 50 mK–6 K temperature range by optically modifying the spin populations and monitoring their return to thermal equilibrium via absorption spectroscopy. Below 1 K, population rethermalization occurs on timescales of several hours and is governed by direct spin-phonon relaxation. In contrast, the lifetime of individual spin states is strongly reduced by spin-spin interactions, ranging from seconds in low-doped (2 ppm) samples to milliseconds at higher doping (10 ppm). These results provide clear guidelines for optimizing doping concentration and operating temperature, indicating that atomic frequency comb lifetimes on the order of one hour are achievable in 171 Yb:Y 2 SiO 5 crystals with Yb concentrations not much lower than 2 ppm and at temperatures at or below 1 K.
Advanced applications of quantum information science, such as long-distance quantum communication based on quantum repeaters, require photons to be interfaced with different devices. These devices, such as single photon detectors, quantum memories, quantum signal processors, and linear optical elements, may be integrated on a single chip to enable efficient, robust and scalable implementations. With aim of constructing a quantum repeater, and towards realizing integrated optical quantum memories and signal processors in general, we experimentally develop quantum light-matter interfaces using a cryogenically-cooled rare-earth-ion-doped waveguide, namely thulium-doped lithium niobate (Tm3+:LiNbO3). As the basis for our work, we describe a quantum repeater architecture that uses spectral multiplexing and quantum memories that operate with a fixed storage time. Our repeater architecture promises efficient operation, is compatible with the properties of cryogenically-cooled rare-earth-ion-doped crystals, and simplifies the demands of quantum memories compared to other architectures. To demonstrate the feasibility of our repeater design, we utilize our light-matter interface as a quantum memory to perform several experimental demonstrations. These include high-fidelity storage and retrieval of 26 spectrally-multiplexed quantum bits encoded into single-photon-level laser pulses, high-fidelity storage and retrieval of single and entangled photons derived from a photon-pair source, and high-visibility two-photon interference between weak laser pulses that are stored in one or two, separate, quantum memories. The unique properties of our light-matter interface allow us to demonstrate additional protocols that further highlight its promise for integrated quantum signal processing. By combining our Tm3+:LiNbO3 waveguide with a LiNbO3 waveguide phase modulator, we demonstrate operations such as sequencing, filtering, interference, and compression of laser pulses attenuated to the single-photon level. In another experiment, we measure the cross-phase modulation between strong pulses, by which we demonstrate photon-photon interactions that point towards non-destructive measurements of quantum bits. Since the performance of all aforementioned protocols, and future light-matter applications, hinge on the basic spectroscopic properties of our waveguide, we measure these properties at temperatures as low as 800 millikelvin. Our findings, discussed over several attached publications, usher the development of integrated quantum memories and processors for multi-component optical quantum information applications such as repeaters and networks.