Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC)
A Pathway to Er Sites in Si with Long Spin and Optical Coherence Times
Alexey Lyasota, Ian R. Berkman, Gabriele G. de Boo, John G. Bartholomew, Brett C. Johnson, Jeffrey Colin McCallum, Bin-Bin Xu, Shouyi Xie, Rose L. Ahlefeldt, Matthew J. Sellars, Chunming Yin, Sven M. J. Rogge
Rare-earth ions in solid-state hosts exhibit low homogeneous broadening and long spin coherence at cryogenic temperatures thus making them a promising candidate for optical quantum memories [1], optical-microwave transducers [2] and single dopant-based devices such as single photon emitters operating at the telecommunication wavelengths [3]. Here, we present an overview of the spin and optical properties of Er ensembles in Si accessed via resonant photoluminescence excitation (PLE) spectroscopy [4]. Samples were positioned directly on top of tailor-fabricated superconducting single photon detectors, placed in a dilution refrigerator unit and resonantly excited using fiber optics. Our method provided high collection efficiency and allowed spectral measurements of low Er density samples. The observed Er PLE spectra were strongly affected by the presence of co-dopants such as O, B or P reflecting their influence on the formation of optically active Er sites and corresponding Er optical transition energies. Higher O densities resulted in especially rich PLE spectra suggesting that a variety of Er-O complexes formed due to O doping. Lowering the O concentration, we achieved PLE spectra dominated by a single Er site in P doped samples. Interestingly, the Er spin relaxation and optical coherence properties were barely affected by the employed co-dopants and mainly depended on the Er concentration. By lowering the Er concentration from relatively high (1018cm-3) to low densities (1016cm-3), we were able to increase Er spin lifetimes from ~0.1 s to ~30 s. Long spin relaxation times allowed us to identify PLE spectra of new Er sites in Si. In both concentration regimes, we observed sub-MHz transient spectral holes suggesting long optical coherence times. Furthermore, we observed sub-MHz spin transitions in both natural and isotopically purified Si and achieved spin coherence times above 1 ms in isotopically purified Si. Narrow optical linewidths and long transverse and longitudinal spin relaxation times show that Er in Si is an excellent candidate for future quantum information and communication applications.
Rare-earth ions in solid-state hosts exhibit low homogeneous broadening and long spin coherence at cryogenic temperatures thus making them a promising candidate for optical quantum memories [1], optical-microwave transducers [2] and single dopant-based devices such as single photon emitters operating at the telecommunication wavelengths [3]. Here, we present an overview of the spin and optical properties of Er ensembles in Si accessed via resonant photoluminescence excitation (PLE) spectroscopy [4]. Samples were positioned directly on top of tailor-fabricated superconducting single photon detectors, placed in a dilution refrigerator unit and resonantly excited using fiber optics. Our method provided high collection efficiency and allowed spectral measurements of low Er density samples. The observed Er PLE spectra were strongly affected by the presence of co-dopants such as O, B or P reflecting their influence on the formation of optically active Er sites and corresponding Er optical transition energies. Higher O densities resulted in especially rich PLE spectra suggesting that a variety of Er-O complexes formed due to O doping. Lowering the O concentration, we achieved PLE spectra dominated by a single Er site in P doped samples. Interestingly, the Er spin relaxation and optical coherence properties were barely affected by the employed co-dopants and mainly depended on the Er concentration. By lowering the Er concentration from relatively high (1018cm-3) to low densities (1016cm-3), we were able to increase Er spin lifetimes from ~0.1 s to ~30 s. Long spin relaxation times allowed us to identify PLE spectra of new Er sites in Si. In both concentration regimes, we observed sub-MHz transient spectral holes suggesting long optical coherence times. Furthermore, we observed sub-MHz spin transitions in both natural and isotopically purified Si and achieved spin coherence times above 1 ms in isotopically purified Si. Narrow optical linewidths and long transverse and longitudinal spin relaxation times show that Er in Si is an excellent candidate for future quantum information and communication applications.
This thesis investigates the potential of Er:YSO and Er:Si for quantum communication and computation applications. Erbium uniquely possess optical transitions in the 1.5 um region, making it suitable for both fibre telecommunication and silicon photonics. The properties of the I15/2↔I13/2 optical transition in Er:YSO have already been extensively studied. Over two decades ago, improvements in Er3+ dephasing time at 1.5 um were achieved by applying a 5T field along the D1 axis. More recently, a record 4.4 ms coherence time on the same optical transition was achieved using a 7T field. These investigations, among others, illustrate that large Er electron spins become thermally polarised with sufficient magnetic field. However, no long lived and coherent spin transitions associated with the Er ions had previously been identified, and such transitions are necessary for on-demand quantum state storage. To address this requirement, the optical and hyperfine transition properties of 167-Er:YSO were investigated in large magnetic fields. In a field of 7T, spectral hole lifetimes of 1 minute and hyperfine population lifetimes of 12 minutes were observed. These measurements illustrate the effect of spin-lattice relaxation in this system, and how it can be mitigated. Efficient spin-polarisation of the entire 167-Er hyperfine ensemble is also demonstrated. This is the first such demonstration in rare earth systems, and a key requirement for broadband optical storage. Moreover, a 1.3 second coherence time was recorded for an 167-Er:YSO hyperfine transition at 7T and 1.4 K. This is an improvement of several orders-of-magnitude over previous coherence measurements on spin-transitions in Er doped solids. This is also sufficient for maximal entanglement rates in quantum repeater networks that span distances of 1000 km or greater. With an optical transition at 1.5 um, Er is also an ideal candidate to connect silicon based quantum computers to the future quantum Internet. In particular, single Er:Si ions could be used to develop an optical-spin bus between P:Si qubits and fibre based quantum networks. Presented here is the first spectroscopic investigation of single Er:Si ions. This required a novel opto-electronic approach to single ion detection, where the Er ions are implanted into a nanometre scale fin-shaped Field Effect Transistor. With this approach it was possible to develop high resolution optical spectra, where both the electronic and hyperfine levels of individual Er ions were resolved. Long optical and spin coherence times are also important requirements for an optical-spin bus. To address the first requirement, an investigation of the optical lineshape was undertaken. Here it was determined that sources of Stark noise external to the transistor channel contribute a significant amount to optical homogeneous linewidth. However, the dominant noise contribution was determined to be short-range (from within the 30 nm wide channel) and the total homogeneous linewidth was measured to be 50 MHz. The site structure of an individual Er:Si ion was then analysed, using magnetic field rotation patterns and optical transitions between multiple crystal field levels. This site was determined to have approximately axial (C3) symmetry. The purpose of this study was to determine a magnetic field regime in which the Er electrons spin can be polarised, which is necessary for realising of long hyperfine lifetimes and coherence times.
Clock-transition-enabled long electron spin coherence of telecom emitters in CeO2
Rare-earth-ion-doped crystals has emerged as a promising platform for quantum technologies, owing to their narrow telecom-band optical emission, long spin memory, and compatibility with silicon integrated photonic architectures. However, the realization of scalable quantum devices requires host materials with intrinsically dilute spin environments to suppress decoherence. In this context, erbium (Er3+) doped cerium oxide (CeO2) is an attractive candidate due to the ultra-low concentration of nuclear spins in the host matrix and its compatibility with silicon-based technologies. Here we perform a comprehensive investigation of the coherence properties of Er3+ electron spin qubit in CeO2 via semiclassical as well as detailed cluster correlation expansion simulations. By systematically exploring magnetic field strength, pulse sequences, erbium concentration, and spin temperature, we identify regimes where decoherence from the spin bath is strongly suppressed. Our investigations illustrate that at dilute doping concentration (of the order of 10 ppb) and sub-Kelvin temperatures, operation near clock transitions enables Hahn-echo coherence times to approach the second timescale even at natural isotopic abundance. Importantly, from a practical standpoint, coherence times on the order of ∼10 ms are expected even at liquid helium temperature (about 2 K) for similar concentrations. Moreover, we demonstrate that an additional enhancement can be obtained with conventional multi-π-pulse dynamical decoupling protocols. Thus, our findings establish Er3+ doped CeO2 as a front-runner for realizing spin qubits, quantum memories, and integrated quantum networks.
Rare-earth ion dopants in solid-state hosts are ideal candidates for quantum communication technologies, such as quantum memories, due to the intrinsic spin–photon interface of the rare-earth ion combined with the integration methods available in the solid state. Erbium-doped cerium oxide (Er:CeO2) is a particularly promising host material platform for such a quantum memory, as it combines the telecom-wavelength (∼1.5μm) 4f–4f transition of erbium, a predicted long electron spin coherence time when embedded in CeO2, and a small lattice mismatch with silicon. In this work, we report on the epitaxial growth of Er:CeO2 thin films on silicon using molecular beam epitaxy, with controlled erbium concentration between 2 and 130 parts per million (ppm). We carry out a detailed microstructural study to verify the CeO2 host structure and characterize the spin and optical properties of the embedded Er3+ ions as a function of doping density. In as-grown Er:CeO2 in the 2–3 ppm regime, we identify an EPR linewidth of 245(1) MHz, an optical inhomogeneous linewidth of 9.5(2) GHz, an optical excited state lifetime of 3.5(1) ms, and a spectral diffusion-limited homogeneous linewidth as narrow as 4.8(3) MHz. We test the annealing of Er:CeO2 films up to 900 °C, which yields narrowing of the inhomogeneous linewidth by 20% and extension of the excited state lifetime by 40%.
We present a flexible method to study the optical properties of an Er3+ ensemble in Si accessed via resonant excitation and in situ single-photon detection. The technique allows an efficient resonant photoluminescence detection of optically active centers with weak oscillator strength in transparent crystals without the need for nanofabrication on the sample. We observe 70 Er3+ resonances in Si, of which 62 resonances have not been observed in the literature, with optical lifetimes ranging from 0.5 to 1.5 ms. We observe inhomogeneous broadening of less than 400 MHz and an upper bound on the homogeneous linewidth of 0.75 and 1.4 MHz for two separate resonances. These narrow, stable resonances confirm Er3+ in Si as a promising quantum information candidate. We discuss the use of this technique for rapid characterization of future samples, with the aim of enhancing the prevalence of sites which are favorable for quantum information applications.
Isotopically enriched epitaxial CaWO4 thin films for Er3+ spin-photon quantum interfaces
Rare earth ion (REI)-doped oxide thin films are attractive for the application of quantum interconnects due to their stable optical levels and scalability1−3. Among them, Er3+ doped CaWO4 is promising because it possesses narrow optical linewidth transitions and a long spin coherence time4−6. The electron spin coherence is limited at high temperatures by paramagnetic impurities and by the presence of the 14.3% 183W nuclear spin. To further increase the spin coherence time at millikelvin temperatures, where the paramagnetic impurities are frozen out, our approach is to synthesize chemically and isotopically purified thin films as a host material. We first grow non-isotopically enriched Er3+ doped CaWO4 thin films, which exhibit a 214(13) MHz photoluminescence (PL) inhomogeneous linewidth, indicating the thin film has high crystalline quality. We then grow isotopically enriched CaWO4 thin films using an isotopically purified 186WO3 source. Time of flight secondary ion mass spectrometry (ToF-SIMS) was used to measure the relative concentration of W isotopes. 183W, the only W isotope that has a net nuclear spin and is the major cause of spin decoherence, was at a relative abundance of 1.2%, a factor of 10 lower than natural abundance. We also observed PL emission from single ions after integrating nano-photonic devices with the thin film. These results establish isotopically engineered CaWO4 thin films as a promising platform for future studies of nuclear-spin-limited coherence and for scalable rare-earth-ion-based quantum nanophotonic devices.
Rare-earth ions (REIs) have incomplete 4f shells and possess narrow optical intra-4f transitions due to shielding from electrons in the 5s and 5p orbitals, making them good candidates for solid-state optical quantum memory. The emission of Er3+ in the telecom C-band (1530 nm–1565 nm) makes it especially attractive for this application. In order to build practical, scalable devices, the REI needs to be embedded in a non-interacting host material, preferably one that can be integrated with silicon. In this paper, we show that Er3+ can be isovalently incorporated into epitaxial Y2O3 thin films on Si (111). We report on the synthesis of epitaxial, single-crystalline Er:Y2O3 on Si with a narrow inhomogeneous linewidth in the photoluminescence (PL) spectra, 5.1 GHz (<100 mK), and an optical excited state lifetime of 8.1 ms. The choice of Y2O3 was driven by its low nuclear spin and small lattice mismatch with Si. Using PL and electron paramagnetic resonance, we show that Er3+ substitutes for Y in the crystal lattice. The role of interfacial SiOx, diffusion of silicon into the film, and the effect of buffer layers on the inhomogeneous PL linewidth are examined. We also find that the linewidth decreased monotonically with film thickness but surprisingly exhibits no correlation with the film crystalline quality, as measured by the x-ray rocking curve scans, suggesting other factors at play that limit the inhomogeneous broadening in Y2O3 films.