Rare-earth-doped crystals are promising candidates for quantum storage, yet their performance in free-space configurations is fundamentally restricted by low optical depth. Here, we demonstrate high-efficiency quantum storage in a stoichiometric EuCl$_3 \cdot$ 6D$_2$O crystal, which intrinsically provides high optical density without the complexity of cavity implementation. We show that in this high-density regime, the system exhibits significant slow-light-like effects, including dispersion-induced echo delays and finesse-dependent echo intensity modulation. We develop a unified theoretical framework showing how absorption and dispersion work in concert to mediate echo generation. We achieve storage efficiencies of 42.9% for classical light and 34.4% for weak coherent pulses, alongside 90% efficiency for slow-light storage. These findings validate EuCl$_3 \cdot$ 6D$_2$O as a robust platform, establishing a viable pathway for scalable solid-state quantum memory.
Slow-light-enhanced Atomic Frequency Comb Quantum Memory in Stoichiometric EuCl3⋅ 6D2O
Rare-earth-doped crystals are promising candidates for quantum storage, yet their performance in free-space configurations is fundamentally restricted by low optical depth. Here, we demonstrate high-efficiency quantum storage in a stoichiometric EuCl3⋅ 6D2O crystal, which intrinsically provides high optical density without the complexity of cavity implementation. We show that in this high-density regime, the system exhibits significant slow-light-like effects, including dispersion-induced echo delays and finesse-dependent echo intensity modulation. We develop a unified theoretical framework showing how absorption and dispersion work in concert to mediate echo generation. We achieve storage efficiencies of 42.9% for classical light and 34.4% for weak coherent pulses, alongside 90% efficiency for slow-light storage. These findings validate EuCl3⋅ 6D2O as a robust platform, establishing a viable pathway for scalable solid-state quantum memory.
When doped into solid state transparent crystals, rare-earth ions can have optically excited states with milliseconds coherence time and up to six hours coherence time for hyperfine levels after being cooled down to liquid helium temperature. This long coherence property makes them unique as solid state material and attractive for quantum information applications.The rare-earth ions have narrow homogeneous linewidths on the order of ~ kHz. When doped into a crystal, the lattice structure is slightly distorted due to the size mismatch between the dopant and the host ions, resulting in slight differences in the local crystal fields at the dopant sites. Therefore, the resonance frequencies of the rare-earth ions are shifted relatively, resulting in an inhomogeneously broadened absorption profile, typically on the order of a few GHz. This provides the possibility of addressing each group of ions individually and engineering the absorption profile for different purposes by optical pumping using a narrow linewidth laser, and makes rare-earth-ion-doped crystals suitable for ensemble based quantum memories.Quantum memories are vital components for developing longdistance quantum communication. Part of this thesis project focused on making quantum memories with high efficiency and long storage time, especially using materials with low optical depth. To achieve this goal, a low finesse, unsymmetrical cavity was employed and experiments were carried out at (or close to) the impedance matched condition. Atomic frequency comb (AFC) protocol proposed for such an inhomogeneously broadened system was used to store coherent light for a certain time. 56% overall efficiency was achieved, and the main limiting factor for reaching even higher efficiency was the inefficient coupling between incoming light and the cavity mode. Other possible loss mechanisms were analyzed as well.Long-time, on-demand, quantum memory experiments were conducted with the help of two efficient radio-frequency rephasing pulses. Storage time was extended from microseconds to milliseconds after compensating (most of) the residual earth magnetic field in the lab. The opportunities and challenges of combing the cavity assistant quantum memory and the long time, on demand quantum memory were analyzed and possible solutions were proposed. Another part of the thesis project involves slow light-based applications in rare-earth-ion-doped crystals. The strong slow light effect at the presence a spectral hole is due to the fact that the light interacts with the absorbing ions outside the spectral hole off-resonantly, and most of the light energy is stored inside the ions as a polarization. For example, with a group velocity of 300 km/s, 99.9% of the pulse energy is stored in the ions when the pulse propagates inside the crystal. The slower the light propagates, the more energy is stored inside the medium. Based on this, a frequency shifter that is capable of shifting the light frequency of ± 4 MHz was demonstrated, and frequency shift up to GHz was proposed. Group velocity control by a factor of 20 and pulse compression in time by a factor of 2 were also demonstrated. The frequency shift and group velocity of the light are solely controlled by the external electric field, which makes them ideal for weak light situation. The unique property of such a frequency shifter and group velocity controller is that they could be made to accept light from an arbitrary incoming angle and polarization, for example, scattered light.
The main aim of the present thesis is to demonstrate the efficient quantum memories for light employing coherent processes in rare-earth-ion-doped crystals. Rare-earth (RE) ions between lanthanum, with atomic number 57, and lutetium, with atomic number 71, have a partly filled 4f shell, which is spatially inside the full shells 5s, 5p, and 6s. Therefore, 4f-4f transitions are shielded from environmental noise. Less noise means longer lifetime and coherence times and, when the crystals are cooled down to about 4 K, these can be about 8 orders of magnitude longer than what is typical for electronic transitions in solids. In quantum information processing, we are looking for physical systems which are isolated from the environment and consequently have good coherence properties. The long coherence time of both optical and spin transitions, is the main attraction of rare-earth ions for quantum information processing. In the present thesis, we map a quantum state of light employing a 4f-4f transition of praseodymium doped in yttrium silicate. We mainly employed the ensemble approach and the atomic frequency comb (AFC) protocol for quantum memory demonstrations. Among several parameters that define quantum memory performance, we mostly focused on quantum memory efficiency. The overall memory efficiency is simply defined as the energy of the pulse recalled from the memory divided by the energy of the pulse sent in for storage in the memory. To maximize quantum memory efficiency, most protocols require high optical depth. This is a limitation for materials with rather good coherence properties but low optical depth. In the research described in the present thesis, we combined the use of a low finesse cavity and the ensemble approach and designed an impedance-match cavity to obtain the advantages of both approaches and thereby to implement an efficient quantum interface in a weakly absorbing solid-state medium. Based on the cavity configuration, we obtained 56% storage and retrieval efficiency, which is the highest storage and retrieval efficiency based on the AFC protocol reported in the research so far. In the present thesis, we demonstrated a narrow-band (about 2 MHz) spectral filter with a >30 dB intensity absorption/transmission ratio, which is based on the large (6 orders of magnitude) ratio between the inhomogeneous and homogeneous broadening of Pr3+ : Y2SiO5. Slow-light effects due to the strong dispersion created by the spectral filter improved the suppression of the filter by also utilizing the time domain. As an application, we detected weak diffuse light shifted by ultrasound from the carrier about 2 MHz, after a 9 cm thick biological tissue. The coupling between light and matter is directly related to the relative direction of the light polarization and transition dipole moment of atoms. I developed a simulation program that was able to investigate the polarization direction and ellipticity of polarization of optical radiation propagating through the crystal. This might open up new opportunities for the investigation of interesting physics regarding propagation effects and for the improvement of spectral engineering of RE ions in the future. In order to deal with the sharp homogeneous transitions of the RE ions, the frequency of our dye laser was stabilized against a highly stabilized Fabry-Perot cavity using the Pound-Drever-Hall locking scheme.
High-efficiency optical storage in rare-earth-ion-doped crystals is challenging because of their typically weak optical absorption,which makes cavity-enhanced memories highly sensitive to parasitic intracavity loss. Here we demonstrate a 90.1(5)% storage efficiency for coherent optical pulses in an impedance-matched cavity atomic-frequency-comb memory based on Eu3+:Y2SiO5. The Brewster-angle configuration of the crystal and fully cryogenic Fabry-Pérot cavity reduce the round-trip intracavity loss to 0.37%. Quantitative modeling shows that further improvement is limited primarily by AFC preparation and its associated dispersive response rather than by residual cavity loss,identifying the principal requirements for further approaching unity efficiency.
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.
We report on the experimental demonstration of an optical spin-wave memory, based on the atomic frequency comb (AFC) scheme, where the storage efficiency is strongly enhanced by an optical cavity. The cavity is of low finesse, but operated in an impedance matching regime to achieve high absorption in our intrinsically low-absorbing Eu 3+ :Y 2 SiO 5 crystal. For storage of optical pulses as an optical excitation (AFC echoes), we reach efficiencies of 53% and 28% for 2 μ s and 10 μ s delays, respectively. For a complete AFC spin-wave memory we reach an efficiency of 12%, including spin-wave dephasing, which is a 12-fold increase with respect to previous results in this material. This result is an important step towards the goal of making efficient and long-lived quantum memories based on spin waves, in the context of quantum repeaters and quantum networks.
Quantum memories are a key building block for optical quantum computers and quantum networks. Rare-earth ion-doped crystals are a promising material to achieve quantum memory using an atomic frequency comb protocol. However, current atomic frequency comb memories typically use bulk materials or waveguides with large cross sections or rely on fabrication techniques not easily adaptable to wafer scale processing. Here, we demonstrate a compact chip-integrated atomic frequency comb in rare-earth-doped thin-film lithium niobate. Our optical memory exhibits a broad storage bandwidth exceeding 100 MHz and optical storage time as long as 250 ns. The enhanced optical confinement in this device leads to three orders of magnitude reduction in optical power required for a coherent control as compared to ion-diffused waveguides. These compact atomic frequency comb memories pave the way toward scalable, highly efficient, electro-optically tunable quantum photonic systems that can store and manipulate light on a compact chip.