Optical waveguides in rare-earth-doped crystals are one of the most promising systems for practical implementations of quantum memory. To further develop these systems, detailed understanding of these materials is required. We report experimental studies of the optical properties and decoherence for Tm3+:LiNbO3, Pr3+:LiNbO3, Er3+:LiNbO3 and Er3+:KTiOPO4 (KTP) bulk crystals for quantum memory applications and discuss potential differences between the properties of the bulk single crystals and optical waveguides. These systems include the rare-earth ions most commonly exploited in quantum memory studies incorporated into two of the most technologically significant waveguide host materials. Photon echo methods were used to study decoherence as a function of temperature, applied magnetic field strength, dopant concentration and excitation wavelength. Decoherence mechanisms were investigated and modelled to interpret the observed behaviour. Spectral hole burning was used to characterize Stark and Zeeman effects. Bulk crystal properties were compared and contrasted to the properties of doped waveguides.
Optical waveguides in rare-earth-doped crystals are one of the most promising systems for practical implementations of quantum memory. To further develop these systems, detailed understanding of these materials is required. We report experimental studies of the optical properties and decoherence for Tm3+:LiNbO3, Pr3+:LiNbO3, Er3+:LiNbO3 and Er3+:KTiOPO4 (KTP) bulk crystals for quantum memory applications and discuss potential differences between the properties of the bulk single crystals and optical waveguides. These systems include the rare-earth ions most commonly exploited in quantum memory studies incorporated into two of the most technologically significant waveguide host materials. Photon echo methods were used to study decoherence as a function of temperature, applied magnetic field strength, dopant concentration and excitation wavelength. Decoherence mechanisms were investigated and modelled to interpret the observed behaviour. Spectral hole burning was used to characterize Stark and Zeeman effects. Bulk crystal properties were compared and contrasted to the properties of doped waveguides.
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.
This thesis presents a spectroscopic study of Pr3+ ions in a novel passive waveguide architecture. To make this structure, the high refractive glass TeO2 was selected as the thin film and it was deposited on a Pr3+:Y2SiO5 crystal. In this waveguide, the 3H4 to 1D2 transition of Pr3+ ions were probed by the optical evanescent field extending into the substrate. The main concern in assessing the suitability of this material for quantum information applications was ensuring that the coherence properties of rare-earth ions, making them suitable for quantum information purposes, are preserved in this architecture. After which, to make low loss devices with these waveguides, efficient coupling techniques had to be developed. To prove that the coherence properties of the rare-earth ion doped crystal were preserved, the critical parameters of inhomogeneous linewidth, the absorption of the ions, the coherence time and spin lifetimes of the Pr3+ ions were studied. The inhomogeneous linewidth of evanescent coupled ions was about 10.0 GHz, which was consistent with the linewidth of bulk samples with the same Pr3+ doping concentration (Hedges, 2011). The absorption due to the evanescent coupling was 9.38 dB, approximately 90% of what was expected with respect to the bulk crystal with the same doping concentration. Therefore, despite using the evanescent field, the absorption is high enough for quantum memory applications. An optical coherence time of about 121 microseconds was measured, which corresponded to a homogeneous linewidth of about 2.6 kHz. This is very close to bulk sample measurements of 111 microseconds, with the same temperature and doping concentration (R. W. Equall, 1995). The spin state lifetime observed was about 9.8 s, which is also very close to the bulk sample measurement of 8.67 s (Mieth, 2016). Initial Stark shifting experiments were performed to determine whether the active ions in the substrate of the passive waveguides could be electrically controlled by applying a small voltage to electrodes on the thin film. In these experiments with a voltage change of 100 mV, the measured holewidth broadening was increasing about 0.55 MHz, which was similar to the calculated values of 0.45 MHz. The Stark coefficient for site 1 was 51.6 kHzcm/V along the D2 axis of the crystal (site 1 will be explained in Section 4.3). (F.R. Graf, 1997). Prism coupling and grating coupling were used to couple light to the ions in the substrate. Prism coupling is an easy and quick method to couple light into a waveguide and observe the properties of the system. However, grating coupling is much more practical when moving towards building a device using this method. The measurements described above indicated that the properties of ions interacting with the evanescent tail of the waveguide mode were consistent with those of bulk ions. This investigation also showed that depositing a glass thin film on a rare-earth ion doped crystal was not affecting the good coherence properties of the substrate. These results establish the foundation for large, integrated, controllable and high performance rare earth ion quantum waveguide systems.
This thesis describes experiments aimed at developing a key component in applications such as quantum networks and long-distance quantum communication systems: quantum memories. Quantum memories for light using photon-echo and coherent rephrasing techniques have been developed. The work is carried out on rare-earth-ion-doped inorganic crystals. Several properties are associated with these crystals such as long coherence times and long-lived ground state sublevels that are particularly interesting in connection applications in the area of quantum information science. It is demonstrated the preparation of optical inhomogeneous absorption profiles such that the light only interacts with a specific transition at a selected frequency. Narrow absorbing structures with widths of <100 kHz have been prepared with no absorption in the surrounding spectral interval. Most of the experiments were carried out using Pr3+:Y2SiO5. However, in our search for suitable a Λ-system in the material under consideration, we also performed spectral hole-burning spectroscopy in Nd:Y2SiVO4. As part of the search for host materials for Pr, Pr:La2(WO4)3 crystal was characterized using a variety of methods, such as, hole burning and photon-echoes. Electromagnetically induced transparency was also observed in this crystal. The most important criteria for evaluating quantum memory performance and the most important physical requirements are discussed. After investigating the standard photon echo techniques and controlled reversible inhomogeneous broadening (CRIB) for quantum state storage, we considered an efficient multimode quantum memory protocol; the atomic frequency comb (AFC) protocol. Combs with peaks of widths 100-300 kHz and an optical depth of~ 10 were created by optical pumping inside an emptied region of the inhomogeneous profile of Pr3+:Y2SiO5, allowing us to improve the efficiency of light storage. Light storage combining a photon-echo technique based on an AFC and spin-wave storage have been demonstrated, and an experimental AFC scheme for the storage of weak coherent light pulses in Pr3+:Y2SiO5 is presented. Finally, we have investigated superradiance and slow light effects. Both these effects occur in the high optical depth regime and can influence the memory performance. Under certain conditions superradiance results in the immediate re-emission of the stored light in a single burst of coherent radiation, and inside spectrally structured materials, slow light effects may result when storage is performed.
Rare-earth-ion doped materials are studied for a quantum information protocol, controlled reversible inhomogeneous broadening, for storing single photons. Coherence properties of Er-doped silicate optical fibers and Er-doped LiNbO3 waveguiding structures are investigated. Spectral hole burning spectroscopy is performed in Erbium and Neodymium doped crystals and spectral tailoring is demonstrated in Nd³?:YVO4. The preservation of information encoded into the relative phase and amplitudes of optical pulses during storage and retrieval in an optical memory based on stimulated photon echo is demonstrated. Furthermore photon echoes stored in spatially separated optical memories in several temporal modes, are retrieved and then combined at a beam splitter. They show almost perfect interference demonstrating both phase preserving storage and indistinguishability of photon echoes. Finally, we report an interference experiment of spontaneous emission of light from two distant solid-state ensembles of atoms and the resulting high fringe visibility implies that the observed spontaneous emission is coherent.
Rare-earth ion ensembles doped in single crystals are a promising materials system with widespread applications in optical signal processing, lasing, and quantum information processing. Incorporating rare-earth ions into integrated photonic devices could enable compact lasers and modulators, as well as on-chip optical quantum memories for classical and quantum optical applications. To this end, a thin film single crystalline wafer structure that is compatible with planar fabrication of integrated photonic devices would be highly desirable. However, incorporating rare-earth ions into a thin film form-factor while preserving their optical properties has proven challenging. We demonstrate an integrated photonic platform for rare-earth ions doped in a single crystalline thin film lithium niobate on insulator. The thin film is composed of lithium niobate doped with Tm 3+ . The ions in the thin film exhibit optical lifetimes identical to those measured in bulk crystals. We show narrow spectral holes in a thin film waveguide that require up to 2 orders of magnitude lower power to generate than previously reported bulk waveguides. Our results pave the way for scalable on-chip lasers, optical signal processing devices, and integrated optical quantum memories.
Efficient and long-lived multimode quantum memories are crucial devices in the development of quantum technolgies. The reversible mapping of quantum states of light in rare earth doped crystals represents one of the most promising routes towards the realization of this goal. Such systems are also compatible with the miniaturization of quantum memories in integrated optics platforms, which offer unique features in terms of experimental scalability and enhanced light-matter interaction. Here, we fabricate single mode channel waveguides for 606 nm light in a praseodymium-doped yttrium orthosilicate crystal (Pr3+:Y2SiO5), that, thanks to its excellent coherence properties, is a widely studied material for light storage experiments. Waveguides are inscribed by femtosecond laser writing, adopting the so-called Type I configuration, where the core is directly obtained at the irradiated area. Remarkably, fabricating this kind of waveguides in crystals is a difficult task, as it requires to operate in a very narrow processing parameters window, if existing. We then use these waveguides for performing the storage and retrieval of single photons, implementing the atomic frequency comb protocol. We achieve a storage time of 5,5 µs, which is almost 2 orders of magnitude longer than previous realizations of quantum light storage in a waveguide. In addition, we investigate the potential information multiplexing capabilities of our system by performing the quantum storage of single photons delocalized over 14 different spectral modes. Our results show that laser written waveguides in rare earth-doped solid state systems are very promising for the development of efficient and long-lived multimode quantum memories.