In this thesis we explore various ways to extend population lifetimes and coherence times of solid-state emitters. We focus on rare-earth-ion doped host materials and silicon vacancy centers in diamond, both of which are used for applications in quantum information processing and quantum communications. Enhanced lifetimes and coherence times would improve the performance of these applications. One approach investigates the possibility to suppress lattice vibrations that cause decoherence and population relaxation by engineering the phonon density of states through nano-structuring of the emitter's host material. Towards this end we study different materials and methods to obtain the desired nano-materials. Using various optical spectroscopic methods, we show that population dynamics can indeed be influenced by modifying the structure of the surrounding host material. However, we also find that the employed fabrication and synthesis methods often induce crystal damage that, in turn, degrades spectroscopic properties. As a second approach, we study rare-earth-ions in disordered host materials. Detailed spectroscopic characterizations are presented and we show with the example of an erbium doped fiber that such materials can indeed feature better properties, specifically longer population lifetimes, than the commonly used bulk crystals. We found optimal operation parameters for the erbium doped fiber which made it possible to use this medium for successful proof of principle experiments demonstrating a multimode quantum memory that operates within the convenient telecom band (around 1550 nm wavelength). Besides increasing the fundamental knowledge, the results of the studies presented in this thesis are highly relevant for the fields of quantum communications and quantum information processing since nano-structured materials are beginning to be investigated for on-chip implementations of various applications such as quantum memories and quantum gates. In addition, we found that population dynamics driven by detrimental lattice vibrations can indeed be modified in small powder materials and thus, with improved fabrication techniques, the complete suppression of lattice vibrations should be possible, benefiting a plethora of applications.
In this thesis we explore various ways to extend population lifetimes and coherence times of solid-state emitters. We focus on rare-earth-ion doped host materials and silicon vacancy centers in diamond, both of which are used for applications in quantum information processing and quantum communications. Enhanced lifetimes and coherence times would improve the performance of these applications. One approach investigates the possibility to suppress lattice vibrations that cause decoherence and population relaxation by engineering the phonon density of states through nano-structuring of the emitter's host material. Towards this end we study different materials and methods to obtain the desired nano-materials. Using various optical spectroscopic methods, we show that population dynamics can indeed be influenced by modifying the structure of the surrounding host material. However, we also find that the employed fabrication and synthesis methods often induce crystal damage that, in turn, degrades spectroscopic properties. As a second approach, we study rare-earth-ions in disordered host materials. Detailed spectroscopic characterizations are presented and we show with the example of an erbium doped fiber that such materials can indeed feature better properties, specifically longer population lifetimes, than the commonly used bulk crystals. We found optimal operation parameters for the erbium doped fiber which made it possible to use this medium for successful proof of principle experiments demonstrating a multimode quantum memory that operates within the convenient telecom band (around 1550 nm wavelength). Besides increasing the fundamental knowledge, the results of the studies presented in this thesis are highly relevant for the fields of quantum communications and quantum information processing since nano-structured materials are beginning to be investigated for on-chip implementations of various applications such as quantum memories and quantum gates. In addition, we found that population dynamics driven by detrimental lattice vibrations can indeed be modified in small powder materials and thus, with improved fabrication techniques, the complete suppression of lattice vibrations should be possible, benefiting a plethora of applications.
This thesis describes a number of coherent processes, such as quantum information processing, superradiance and electromagnetically induced transparency, which have been experimentally implemented using rare-earth-ion-doped crystals. The rare-earths are a class of elements that have in common, an atomic structure that allows for very long lifetimes as well as coherence times, both on optical transitions and on spin transitions. These ions can be naturally trapped inside host crystals, and with the phonon vibrations removed by cooling down to cryogenic temperatures (< 4 K), they can be used for a number of different quantum information processes. Most experiments were carried out using PrYSO, but also other crystal types were investigated, such as Nd:YVO4, and La2(WO4)3. The characterization of the ions were done with a variety of methods, including among others, photon echo techniques and electromagnetically induced transparency. Quantum computing is a rapidly growing field and there are still many potential candidates for its implementation. In our work we have utilized the spin states of the Pr rare-earth ion as a qubit, and demonstrated arbitrary single qubit gates, which are important pieces towards a quantum computing realization in these systems. Most of the experimental work done for the thesis was carried out using an ensemble approach, that has the advantage of giving a strong readout signal, but for future scaling to multiple qubits, single instances are more promising, which is discussed. Quantum memories are crucial components in applications such as quantum networks and long distance quantum communication. In this thesis, work has been done to investigate how quantum memories can be implemented in rare-earth crystals. In particular, there are two protocols, CRIB and AFC, which were suggested with rare-earth crystals directly in mind, and both of these require high optical depth, for maximum recall efficiency. In this thesis, implications of being in the high optical depth regime, with phenomena such as superradiance, a collective effect that could cause the stored light to be immediately reemitted, and slow light effects that come from performing the storage inside spectrally structured materials, were investigated. In order to carry out the phase-sensitive experiments, a laser system with a very narrow linewidth of ~1 kHz at 606 nm was constructed, by locking the laser to a semi-persistent spectral hole. In addition, many experiments required advanced pulse shapes, such as complex sechyp pulses or pulses obtained from optimal control theory. In order to be able to accurately create such shapes, an elaborate system using an arbitrary waveform generator and two well calibrated AOMs, controlled from a computer, was also built.
Rare-earth ion doped crystals possess stable solid state physicochemical properties and long optical coherence time and spin coherence time, thus showing important development prospect in quantum information science and technology area. Investigations on macroscopic bulk rare-earth single crystals have obtained many promising results, especially in the field of optical quantum memory. With the rapid development of quantum information science, a variety of new functions or multifunctional integrations are found in rare earth crystal systems, such as on chip quantum storage, microwave to optical frequency conversion, scalable quantum single photon sources, and quantum logic gates. As a result, beyond the macroscopic bulk rare-earth single crystals, micro/nano-scale rare-earth crystals have received much attention in recent years and they are regarded as promising candidates in highly integrated hybrid quantum systems and miniaturized quantum devices. Moreover, wet chemical method synthesized micro/nano-scale rare-earth crystals have lower growth difficulty and more flexible manipulation in volume, shape and composition. Therefore, exploring high-performance micro/nano-scale rare-earth crystals and precisely manipulating their quantum states have become one of the important directions in today’s quantum information science and technology research. In this review, we first briefly introduce the basic concepts and high resolution spectroscopic techniques that are commonly used in rare earth ion doped crystals for quantum information science and technologies, such as hole burning technique and photon echo technique. Then we summarize comprehensively recent research status and development trends of rare earth ion doped polycrystalline nanoparticles, thin films, single crystal based micro systems, and some other micro/nano-scale rare earth platforms in terms of material fabrication, quantum coherence property, dephasing mechanisms, and also quantum device explorations. The latest research advances in quantum information applications such as quantum storage, quantum frequency conversion, quantum single photon sources and quantum logic gates are given. Finally, we discuss the possible optimization directions and strategies to improve the component design, material synthesis and quantum performance of micro/nano-scale rare earth crystals and their related quantum devices. This review highlights that the micro/nano-scale rare earth crystals may offer many new possibilities for designing quantum light-matter interfaces, thus are promising quantum systems to develop scalable and integrated quantum devices in the future.
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.
In this thesis, aspects of the use of cryogenically cooled rare-earth-ion-doped crystals in the fields of quantum optics and quantum information processing are addressed. The experiments and theoretical considerations referred to in this thesis are based on the coherent transient interaction between light and the ions in the crystals. A photon echo experiment has been performed where faint optical pulses were accumulated in the crystal. In this experiment, the possibility of single photons acting as two of the optical fields in the photon echo process was investigated. Different aspects on the experiment, which can be viewed as delayed self-interference of a single photon, are discussed in this thesis. A scheme for the possible implementation of quantum information processing in rare-earth-ion-doped crystals is presented. A key feature in this scheme is that small groups of ions, which can be optically manipulated and which interact in a controlled way, can be extracted from a collection of randomly positioned ions in the crystal host. Initial experimental investigations of the scheme, indicating the possibility of implementing quantum gates, are also presented in this thesis. In another experiment, the application of magnetic fields of up to 5 T was seen to increase the lifetime of information stored as frequency-dependent modulation of the population of thulium ions doped into a YAG crystal by several orders of magnitude. This mechanism might be useful in data storage and information processing applications. An experiment in which the same type of crystal was used as the active medium in a photon-echo-based pulse compression experiment, where microsecond long pulses were compressed to nanosecond duration using frequency-chirped light pulses, is also reported in this thesis.
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.
Quantum light-matter interfaces that reversibly map the quantum state of photons onto the quantum states of atoms, are essential components in the quantum engineering toolbox with applications in quantum communication, computing, and quantum-enabled sensing. In this talk I present our progress towards developing on-chip quantum light-matter interfaces based on nanophotonic resonators fabricated in rare-earth-doped crystals known to exhibit the longest optical and spin coherence times in the solid state. We recently demonstrated coherent control of neodymium (Nd3+) ions coupled to yttrium orthosilicate Y2SiO5 (YSO) photonic crystal nano-beam resonator. The coupling of the Nd3+ 883 nm 4I9/2-4F3/2 transition to the nano-resonator results in a 40 fold enhancement of the transition rate (Purcell effect), and increased optical absorption (~80%) - adequate for realizing efficient optical quantum memories via cavity impedance matching. Optical coherence times T2 up to 100 μs with low spectral diffusion were measured for ions embedded in photonic crystals, which are comparable to those observed in unprocessed bulk samples. This indicates that the remarkable coherence properties of REIs are preserved during nanofabrication process. Multi-temporal mode photon storage using stimulated photon echo and atomic frequency comb (AFC) protocols were implemented in these nano-resonators. Our current technology can be readily transferred to Erbium (Er) doped YSO devices, therefore opening the possibility of efficient on-chip optical quantum memory at 1.5 μm telecom wavelength. Integration with superconducting qubits can lead to devices for reversible quantum conversion of optical photons to microwave photons.