The effect of instantaneous spectral diffusion (ISD) on gate operations in rare-earth-ion-doped crystals is an important question to answer for the future of rare-earth quantum computing. Here we present a microscopic modeling that highlights the stochastic nature of the phenomenon and use it to investigate ISD errors on single-qubit gate operations. Furthermore, we present a method to estimate the total error from many different error sources by only studying subsystems containing one error source at a time. This allows us to estimate the total ISD error from all nonqubit dopants in the vicinity of a qubit. We conclude that optical pumping techniques must be used to empty the frequency regions around the qubit transitions from absorption (transmission windows) in order to suppress the ISD errors. Despite using such windows, there remains a roughly $0.3%$ risk that a qubit has an ISD error larger than the error from other sources. In those cases, the qubit can be discarded and its frequency channel can be reused by another qubit. However, in most cases the ISD errors are significantly smaller than other errors, thus opening up the possibility to perform noisy intermediate-scale quantum (NISQ) algorithms despite ISD being present.
The effect of instantaneous spectral diffusion (ISD) on gate operations in rare-earth-ion-doped crystals is an important question to answer for the future of rare-earth quantum computing. Here we present a microscopic modeling that highlights the stochastic nature of the phenomenon and use it to investigate ISD errors on single-qubit gate operations. Furthermore, we present a method to estimate the total error from many different error sources by only studying subsystems containing one error source at a time. This allows us to estimate the total ISD error from all nonqubit dopants in the vicinity of a qubit. We conclude that optical pumping techniques must be used to empty the frequency regions around the qubit transitions from absorption (transmission windows) in order to suppress the ISD errors. Despite using such windows, there remains a roughly 0.3 risk that a qubit has an ISD error larger than the error from other sources. In those cases, the qubit can be discarded and its frequency channel can be reused by another qubit. However, in most cases the ISD errors are significantly smaller than other errors, thus opening up the possibility to perform noisy intermediate-scale quantum (NISQ) algorithms despite ISD being present.
Quantum computers based on rare-earth-ion-doped crystals show promising properties in terms of scalability and connectivity if single ions can be used as qubits. Through simulations, we investigate gate operations on such qubits. We discuss how gate and system parameters affect gate errors, the required frequency bandwidth per qubit, and the risk for instantaneous spectral diffusion (ISD). Furthermore, we examine how uncertainties in the system parameters affect the gate errors, and how precisely the system needs to be known. We find gate errors for arbitrary single-qubit gates of $2.1\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}4}$ when ISD is not considered and $3.4\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}4}$ when we take heed to minimize it. Additionally, we construct two-qubit gates with errors ranging from $5\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}4}\ensuremath{\rightarrow}3\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}3}$ over a broad range of dipole-dipole interaction strengths.
In this thesis, crystals of yttrium orthosilicate (Y2SiO5) that are randomly doped with another rare-earth element, such as praseodymium (Pr), europium (Eu), or cerium (Ce), are investigated with lasers locked to ultra-stable cavities using the Pound-Drever-Hall locking technique. Many of these rare-earth elements have long-lived 4f-4f transitions, hundreds of microseconds to a few milliseconds, with even longer ground hyperfine lifetimes of up to several days. The coherence properties are, to the best of the author's knowledge, the longest achieved for any material, currently with a record of six hours for the nuclear spin states of Eu3+:Y2SiO5 measured at cryogenic temperatures. Furthermore, due to natural trapping and differences in the local environments, each dopant ion experiences a slightly different crystal field, and thus an inhomogeneity in the 4f-4f transition exists between all ions in a crystal. Since the homogeneous linewidth is in the order of kHz or below, whereas the inhomogeneous profile can be several GHz wide, these materials have dense storing capabilities.This thesis explores how light interacts with such rare-earth-ion-doped crystals; how the absorption and light polarization varies during propagation; how spectral features in the inhomogeneous absorption profile can be tailored to create narrowband spectral filters; how the speed of light is slowed down significantly in such narrow transmission windows; and how that can be used to either frequency shift incoming light, control its group velocity, or temporally compress pulses. It also uses rare-earth-ions to research quantum computing, the field of using quantum mechanical effects such as superpositions and entanglements to outperform classical computers on certain specific problems. This is done by examining how two-color pulses can be used to rapidly induce coherence from an initially mixed state; how qubit-qubit interactions can be performed experimentally using ensemble qubits, which opens the door to two-qubit experiments such as the CNOT-gate and entanglements; how a scalable quantum computer might be constructed using a single ion qubit approach with a dedicated readout ion and buffer ion(s) to improve readout fidelity; and how cerium is investigated as a candidate for such a dedicated readout ion.
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.
In optically controlled quantum computers it may be favorable to address different qubits using light with different frequencies, since the optical diffraction does not then limit the distance between qubits. Using qubits that are close to each other enables qubit-qubit interactions and gate operations that are strong and fast in comparison to qubit-environment interactions and decoherence rates. However, as qubits are addressed in frequency space, great care has to be taken when designing the laser pulses, so that they perform the desired operation on one qubit, without affecting other qubits. Complex hyperbolic secant pulses have theoretically been shown to be excellent for such frequency-addressed quantum computing [I. Roos and K. Molmer, Phys. Rev. A 69, 022321 (2004)]---e.g., for use in quantum computers based on optical interactions in rare-earth-metal-ion-doped crystals. The optical transition lines of the rare-earth-metal-ions are inhomogeneously broadened and therefore the frequency of the excitation pulses can be used to selectively address qubit ions that are spatially separated by a distance much less than a wavelength. Here, frequency-selective transfer of qubit ions between qubit states using complex hyperbolic secant pulses is experimentally demonstrated. Transfer efficiencies better than 90% were obtained. Using the complex hyperbolic secant pulses it was also possible to create two groups of ions, absorbing at specific frequencies, where 85% of the ions at one of the frequencies was shifted out of resonance with the field when ions in the other frequency group were excited. This procedure of selecting interacting ions, called qubit distillation, was carried out in preparation for two-qubit gate operations in the rare-earth-metal-ion-doped crystals. The techniques for frequency-selective state-to-state transfer developed here may be also useful also for other quantum optics and quantum information experiments in these long-coherence-time solid-state systems.
This thesis work contributes to the effort of detecting single rare earth ions doped into crystals, an operation crucial for the development of rare earth quantum computer hardware. Doping crystals with rare earth elements, their trivalent ions substitute some of the crystal’s original bonds. These ions have a partially filled 4f shell, protected by the full 5s and 5p shell from the environment which makes them good candidates for qubits. Because not every ion experiences the same electric field from the imperfect crystal, their total linewidth is inhomogeneously broadened. If the doping is sufficiently low and the crystal sufficiently small, each ion undergoes a different optical shift and can thus be addressed separately. Communication between ions happens due to their permanent dipole moments which change according to their energy level. So far no single ions could be detected in Lund because highly doped bulk crystals were used. It was nevertheless tried to construct quantum logic gates using qubits that consisted of an ensemble of ions. Constructing logic gates with these means that every single ion of one qubit needs to be able to communicate with every single ion of another qubit, a method that becomes increasingly difficult when more and more qubits are to be entangled. Connecting as many qubits as possible is a crucial step in building a quantum computer that could outperform classical computers and this could be facilitated if every qubit consisted of only one ion which is the reason for the recent explorations towards nano crystals. This development also makes it possible to address another problem of rare earth ions, their low probability of spontaneous emission. Placing nano crystals into an optical cavity promises the enhancement of spontaneous emission by the Purcell effect. Ideal cavities are Fiber Fabry-Pérot resonators of which one side consists of a mirror coated fiber tip and the other of a plane mirror functioning as the substrate for the nano crystals. It was the aim of this thesis to build a cryostat holder that would bring these two mirrors together with high stability and would allow for vertical and horizontal scanning.