Rare earth ions in solids offer optical linewidths rivaling those of trapped single atoms. We design and characterize rare-earth-doped crystals for applications requiring long optical decoherence times (4.2 ms) and ultranarrow spectral holes (75 Hz).
Unique spectroscopic properties of isolated rare earth ions in solids offer optical linewidths rivaling those of trapped single atoms and enable a variety of recent applications. We design rare-earth-doped crystals, ceramics, and fibers with persistent or transient "spectral hole" recording properties for applications including high-bandwidth optical signal processing where light and our solids replace the high-bandwidth portion of the electronics; quantum cryptography and information science including the goal of storage and recall of single photons; and medical imaging technology for the 700-900 nm therapeutic window. Ease of optically manipulating rare-earth ions in solids enables capturing complex spectral information in 105 to 108 frequency bins. Combining spatial holography and spectral hole burning provides a capability for processing high-bandwidth RF and optical signals with sub-MHz spectral resolution and bandwidths of tens to hundreds of GHz for applications including range-Doppler radar and high bandwidth RF spectral analysis. Simply stated, one can think of these crystals as holographic recording media capable of distinguishing up to 108 different colors. Ultra-narrow spectral holes also serve as a vibration-insensitive sub-kHz frequency reference for laser frequency stabilization to a part in 1013 over tens of milliseconds. The unusual properties and applications of spectral hole burning of rare earth ions in optical materials are reviewed. Experimental results on the promising Tm3+:LiNbO3 material system are presented and discussed for medical imaging applications. Finally, a new application of these materials as dynamic optical filters for laser noise suppression is discussed along with experimental demonstrations and theoretical modeling of the process.
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 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.
The main aim of this work, was to lay the foundations for the experimental realisation of a quantum mechanical controlled NOT gate in rare-earth-metal-ion-doped crystals. Small amounts of rare-earth elements, added during the growth of some inorganic crystals, will become substituted into the crystal lattice as trivalent ions. The trivalent rare-earth-metal ions between cerium, with atomic number 58, and ytterbium, with atomic number 70, have a partly filled 4f shell, which does not extend spatially outside the full 5s and 5p shells. The 4f vacancies make electronic inner shell transitions possible between spectroscopic 4f terms. Some of these optical transitions have coherence times of the order of milliseconds, when the crystals are cooled down to ~ 4 K. There are several reasons for these extraordinary coherence times, which are approximately 8 orders of magnitude greater than those typical for electronic transitions in solids. The most important one is the cage-like shield which the outer 5s and 5p shells provide for the 4f electrons. Furthermore, since these ions are naturally trapped inside the crystal lattice there is no Doppler broadening of the line-width. The coherence properties of these optical transitions is one of the features that makes these materials attractive for use as a solid-state platform for quantum computing, using these ions as qubits. Another appealing characteristic is the fact that different ions have different optical resonance frequencies, which means that ions belonging to different qubits, which only have nm separation, can still be addressed separately by using different laser frequencies. Since the inter-ion spacing is so small, it is possible to make two ions interact strongly, although they are well shielded, through a permanent dipole-dipole interaction. This interaction can be turned on and off by switching between two different ways of encoding the qubit, a most useful feature. When the qubit is represented as a superposition between two ground state hyperfine levels, the interaction is turned off. The interaction is turned on selectively by transferring this superposition to the optical transition with a pi-pulse, for the specific ions that are to interact. This thesis describes how peaks of ions, absorbing on a single transition, residing in spectral pits with no other ions, have been isolated. It is shown how these ions can be coherently transferred between hyperfine levels via the optically excited state, how the interaction between such peaks of ions representing qubits can be turned on and off, and how subgroups of ions with strong interaction can be distilled out. All the work described here has been performed using the ensemble approach. The ensemble approach will, however, be difficult to scale up to large numbers of qubits. A method employing a single ion in each qubit, using a specialised ion for readout, has therefore also been proposed. The rare-earth-metal-ion-based quantum computing experiments require a laser with coherence properties which at least match those of the material. To this end a frequency stabilisation system was developed for a dye laser. This system uses a transient spectral hole in a rare-earth-metal-ion-doped crystal, of the same kind that is used in the experiments, as frequency reference, and is to the authors knowledge the first demonstration of locking a dye laser to a spectral hole. This system provides a line-width of 1 kHz on a 10 microseconds timescale and a frequency drift below 1 kHz/s.