Rare-Earth (RE) atoms possess a unique atomic energy level structure, leading to excellent electronic and spin coherence properties [1]. Consequently, RE-ion-doped materials are promising candidates for implementing light-matter interfaces for photonic quantum technologies, such as quantum memories. To exploit these properties in quantum technologies, the REs must be hosted in a solid-state material [1]. RE organic molecular crystals offer advantages over the well-known RE-doped inorganic crystals. In organic molecular crystals, RE ions are integral parts of the molecular structure, unlike in inorganic crystals, in which the RE ions are distributed randomly into the crystal lattice structure. This can potentially lead to narrower inhomogeneous broadening. These crystals provide unmatched flexibility in combining with photonic structures and in material composition, allowing the choice of different ligands and point group symmetries around the RE ion [2], [10], [4]. Our research focuses on crystals formed from a molecular complex hosting erbium ions$\lceil{E}r(C_{5}H_{7}O_{2})_{3}(C_{12}H_{8}N_{2})\rceil$. As these crystals have not yet been studied for quantum information purposes, we conducted a series of optical spectroscopy measurements to characterize the platform. We performed absorption measurements and obtained the absorption profiles at room and cryogenic temperatures. The results show a narrow inhomogeneous broadening in samples with different relative concentrations, even at 100%, for which all molecules contain an erbium ion. We measured the lifetime of the second lowest crystal field level of the ground state manifold$(\boldsymbol{30}\ cm^{-1}$above ground state) to be 1.759 seconds. Additionally, we measured the inhomogeneous broadening of the lowest crystal field level versus temperature to investigate the effects of phonon processes. Finally, under an external magnetic field, we observed Zeeman splitting and determined the g-factor to be 3.23 for erbium ions in this molecular complex.
Rare-Earth (RE) atoms possess a unique atomic energy level structure, leading to excellent electronic and spin coherence properties [1]. Consequently, RE-ion-doped materials are promising candidates for implementing light-matter interfaces for photonic quantum technologies, such as quantum memories. To exploit these properties in quantum technologies, the REs must be hosted in a solid-state material [1]. RE organic molecular crystals offer advantages over the well-known RE-doped inorganic crystals. In organic molecular crystals, RE ions are integral parts of the molecular structure, unlike in inorganic crystals, in which the RE ions are distributed randomly into the crystal lattice structure. This can potentially lead to narrower inhomogeneous broadening. These crystals provide unmatched flexibility in combining with photonic structures and in material composition, allowing the choice of different ligands and point group symmetries around the RE ion [2], [10], [4]. Our research focuses on crystals formed from a molecular complex hosting erbium ions⌈Er(C5H7O2)3(C12H8N2)⌉. As these crystals have not yet been studied for quantum information purposes, we conducted a series of optical spectroscopy measurements to characterize the platform. We performed absorption measurements and obtained the absorption profiles at room and cryogenic temperatures. The results show a narrow inhomogeneous broadening in samples with different relative concentrations, even at 100%, for which all molecules contain an erbium ion. We measured the lifetime of the second lowest crystal field level of the ground state manifold(30cm−1above ground state) to be 1.759 seconds. Additionally, we measured the inhomogeneous broadening of the lowest crystal field level versus temperature to investigate the effects of phonon processes. Finally, under an external magnetic field, we observed Zeeman splitting and determined the g-factor to be 3.23 for erbium ions in this molecular complex.
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.
This thesis describes investigations of the use of cryogenically cooled rare-earth-ion-doped crystals for quantum information processing and quantum optics. Several aspects of the coherent interaction between light and rare-earth ions in solids are addressed. Quantum information science has given physicists new views of quantum mechanics. The transmission of quantum states has already found practical use and full scale quantum computers may one day perform computations and simulations that would be impossible on a conventional computer. The work presented in this thesis can be seen as a part of a broad effort to learn how to control and manipulate quantum mechanical systems, which will become necessary as science and technology continue to push ever deeper into the nanoscopic world. Coherent radiation, such as laser light, provides us with an ideal tool for these investigations and, along the way, we may also learn more about the quantum nature of light. Rare-earth ions in inorganic crystals have several unusual properties that are interesting for applications within quantum information science, including long coherence times and long-lived ground state sublevels that can be used for storage of quantum and classical information. As part of the work presented in this thesis, new materials have been investigated with respect to these properties, and ways to enhance the useful properties of the materials were explored. In one investigation, the lifetime of information stored in the ground state population distribution of Tm3 ions in YAG was shown to increase by several orders of magnitude with the application of a magnetic field. It is demonstrated how the optical inhomogeneous absorption profile can be prepared, so that the light only interacts with a selected group of ions, absorbing on a specific transition. Narrow absorbing structures, with widths approaching the optical homogeneous linewidth, have been prepared with no absorption in the surrounding spectral interval. This thesis addresses the use of such structures as hardware for quantum bits. Tailored pulses, capable of inducing controlled changes in the quantum states of the ions (qubits), even in the presence of unknown variations of coupling strengths and frequencies, have been realised experimentally and used for multiple transfer of ions between energy levels. Ion-ion interactions, which can be used for performing quantum logic operations, have been investigated in some detail. Techniques for selecting strongly interacting ions, by transferring weakly interacting ions to auxiliary states, have been demonstrated. A scheme for storing the quantum state of light in a solid, using photon-echo-like techniques, is proposed and analysed. In the proposed scheme, an optical wave packet is absorbed and subsequently re-emitted by an inhomogeneous absorption profile, which is tailored and externally controlled by the application of an electric field Additionally, an accumulated photon echo experiment has been performed using faint optical pulses. The experiment can be viewed as a demonstration of delayed self-interference of a single photon and as a demonstration of how a single photon can act as two of the fields in a photon echo process.
Rare-earth doped insulators have been widely recognized as excellent candidate materials for optical quantum computing and information processing. This is principally due to a combination of optical coherence times of up to milliseconds and ground-state hyperfine coherence times of seconds exhibited by rare-earth 4𝑓 𝑁 states. A key contender among rare-earth doped materials is Er3+:Y2SiO5, for which homogeneous linewidths as narrow as 50 Hz have been reported, and for which transitions between the ground and first excited states fall within the 1.5 𝜇m telecommunications wavelength band. However, attempts to utilize this material for spin-wave storage have been hampered by the complexity of the excited-state hyperfine structure, which inhibits the necessary theoretical work required to predict the location of zero first-order zeeman transitions. To address this, a novel crystal-field fitting method was developed to allow an accurate analysis of the 𝐶1 point-group symmetry sites of Y2SiO5. This work was complemented with spectral hole-burning spectroscopy, which revealed ground-state hyperfine level storage with a lifetime of 1.6 ± 0.4 seconds for the 4I15/2𝑍1 → 4F9/2𝐷1 transition. This type of storage time is uncharacteristic for erbium without an external magnetic field, since spin-flips of the unpaired electron in nearby Er3+ ions are typically understood to lead to fast hole filling. The development process of the theoretical and experimental tools required to perform the above work enabled several additional investigations. In particular, the novel crystal-field fitting methods were applied to the 𝑆4 site of Ce3+:LiYF4 and to the 𝐶2𝑣 site of Sm3+:Na+/Li+:CaF2/SrF2. These studies consisted of excellent tests for the developed methods yet also amounted to interesting investigations in their own respect. Similarly, the experimental work afforded an opportunity to directly determine the hyperfine splittings of the 5I8𝑍1 → 5F5𝐷1 transition in Ho3+:KY3F10. This was achieved using high-resolution excitation spectroscopy. Furthermore, the experimentally determined hyperfine structure could be accurately reproduced using a crystal field model. Finally, a lifetime measurement of the 6H7/2 state of Sm3+:LiYF4 was conducted. By utilizing an infrared free-electron laser, pico-second pump-probe spectroscopy allowed for a direct measurements of one of the shortest lifetimes of an RE3+ doped insulator reported in the literature to date. This confirmed the previously suggested two-gradient modification required for the energy-gap law at very short time scales.
Since quantum information technologies are expected to offer communication security and high computational capacities, research in the field is currently attracting a lot of attention. Among the materials studied so far, rare earth doped inorganic insulators are one of the most promising. With the different available trivalent rare earth ions, the visible and the IR range including the telecom wavelength at 1.5 μm can be covered. Transitions are usually narrow, and at low temperatures, long optical and spin coherence times can often be observed. Investigations using bulk single crystals have already led to many promising results. Recently, spectroscopic studies have been extended to other forms of inorganic materials, such as transparent ceramics, thin films, and nanoparticles for single rare‐earth qubits. Progress in these areas is expected to offer many new possibilities for the design of quantum light‐matter interfaces and scalable quantum memories and processors.
Abstract Doping erbium ions into europium-based hosts offers a promising platform for quantum repeater nodes, combining europium’s exceptional coherence properties for long-term quantum storage with erbium’s microwave compatibility and direct telecom-band emission for efficient optical interfacing. In this work, we investigated erbium-doped EuCl3 · 6H2O stoichiometric crystals as a candidate for such nodes. We demonstrate that erbium doping shifts the optical transition frequencies of nearby Eu3+ ions, producing well resolved satellite lines in the inhomogeneous absorption profile. We experimentally probe the coupling between Er3+ and Eu3+ ions under varying temperature and magnetic field conditions, quantifying the interaction strength, which ranges from tens to hundreds of kilohertz, depending on field orientation, magnitude, and the lattice position of the Eu3+ ions. At 60 mK and a moderate magnetic field of 0.1 T, we observed a strong frozen core effect from Er3+ spins, substantially extending the Eu3+ optical coherence time from 62 us to 162 us, approaching the lifetime limit, and enabling hour-long hyperfine state lifetimes. These results underscore the potential of dual-species rare-earth systems for photonic quantum technologies and highlight their promise for precise quantum control.
Without using any trapping lasers, rare-earth (RE) ions can be doped into some nanofabricated materials in form of nanocrystals in a solid state matrix, thus rendering a natural trap for potential application as a quantum computing device. In particular, passive nuclear spin states of RE ions can be utilized as (i) optical quantum memory (with huge density as yielded from nanocrystals), (ii) qubits by encoding in ground hyperfine states and operated as (iii) two-qubit gate when transferring them to active magnetized electronic states. A feasible implementation of qubits is realised by using those doped RE ions whose open-shell (for inner highly shielded 4f shell electrons) energy levels and statevectors are well described by the crystal field (CF) interaction and hyperfine coupling in which the Hamiltonian is composed of various freeion interactions, the CF potential, electronic and nuclear Zeeman effects as well as the hyperfine interaction. For those qubit encoded in the two ground hyperfine states of RE ions, they can have fairly long lifetimes of days and coherence times (from 1.3s for Er3+ to 6 hours for Eu3+) due to the unique spectroscopic properties of RE ions. Because of the recent progress in optical single-ion detection for addressing individual qubits with a specific frequency channel, RE ions could be packed in a solid state 3D matrix at nanometer spacing, hence rendering very high qubit densities for quantum memories. Meanwhile, this configure also leads to strong dipole-dipole interactions (or high connectivity) between qubits which are not nearest neighbors. In this study, Kramers ions like 167Er and 171Yb doped in yttrium orthosilicate Y2SiO5 (YSO) nanocrystals will be investigated as a promising system for quantum computing because of their weak spin bath and possibility for being directly milled in single nanocrystals as nano-resonators. By using the famous Wien2k package to carry out the first-principles calculations, we can obtain the CF parameters and hyperfine constants as well as various electronic properties like energy gap and band structure for those Kramers RE ions doped in YSO. We shall present some essential findings from first-principles calculations to obtain various properties of the ground and excited CF and hyperfine states for those RE ions with an aim to optimize RE ions doping in YSO nanocrystals for quantum memories and qubits, contributing to scalable quantum computing architectures.