The work presented in this thesis was concerned with investigating the relevant spectroscopic properties of Ce ions randomly doped in an Y2SiO5 crystal at low temperatures (around 4 K), in order to develop a technique and an experimental set-up to detect the fluorescence photons emitted by a single Ce ion. The aim of the work was to determine whether a single Ce ion (referred to as the readout ion) can be used as a local probe to sense the quantum state of a neighbouring single-ion qubit via a state-selective interaction between the readout and qubit ion. More precisely, if the qubit ion is in state |1> or |0> state, the single Ce ion will, or will not, emit fluorescence photons. This single ion readout concept is a key step towards single-rare-earth-ion quantum computing, which is believed to be a promising approach for a scalable quantum computer. Rare-earth ion based quantum computing is an attractive scheme for several reasons. Firstly, the qubit coherence time can be on the timescale of a minute while the optical coherence time can be on the millisecond timescale, despite the fact that the ions are in a solid (crystal), which means that more than 10000 optical pulses could be implemented before the system decoheres. Secondly, any sub-ensemble of ions in a frequency interval equal to or larger than the homogeneous linewidth within the inhomogeneously broadened absorption line can be used as a frequency-selectively addressed qubit. The proof of principle of the qubit-qubit interaction has been previously demonstrated. Thirdly, no special material engineering is required, and the crystal is commercially available. Ways of initializing a sub-ensemble of Pr ions as a qubit in the random system, manipulating the quantum state of the ions in a controlled way, and characterizing the quantum state created are presented. In order to achieve better scalability, the idea of letting a single rare-earth ion represent a qubit was investigated. The fidelity of the single-ion readout scheme was briefly studied. The influence of the energy transfer process between two neighbouring ions on quantum computing is discussed. A readout ion should possess a number of specific spectroscopic properties. Therefore, the position and the linewidths of the zero-phonon line of Ce ions were measured using an external cavity diode laser (at 371 nm) as the excitation source. The difference in the permanent dipole moment of the ground and excited states of Ce ions was measured in a photon echo experiment on Pr ions in a Ce-Pr co-doped Y2SiO5 crystal. The last and most important task was to realize single Ce ion detection. Fluorescence of Ce ions has been detected from a crystal, where there is on average 1 ion within 4.6 \micro m$^3$ interacting with the excitation laser at a time. Estimates were made of the number of ions contributing to an observed signal. A trial experiment to investigate whether the signal was emitted by a single Ce ion was carried out, but was unsuccessful. Potential reasons why the experiment failed are presented.
The work presented in this thesis was concerned with investigating the relevant spectroscopic properties of Ce ions randomly doped in an Y2SiO5 crystal at low temperatures (around 4 K), in order to develop a technique and an experimental set-up to detect the fluorescence photons emitted by a single Ce ion. The aim of the work was to determine whether a single Ce ion (referred to as the readout ion) can be used as a local probe to sense the quantum state of a neighbouring single-ion qubit via a state-selective interaction between the readout and qubit ion. More precisely, if the qubit ion is in state |1> or |0> state, the single Ce ion will, or will not, emit fluorescence photons. This single ion readout concept is a key step towards single-rare-earth-ion quantum computing, which is believed to be a promising approach for a scalable quantum computer. Rare-earth ion based quantum computing is an attractive scheme for several reasons. Firstly, the qubit coherence time can be on the timescale of a minute while the optical coherence time can be on the millisecond timescale, despite the fact that the ions are in a solid (crystal), which means that more than 10000 optical pulses could be implemented before the system decoheres. Secondly, any sub-ensemble of ions in a frequency interval equal to or larger than the homogeneous linewidth within the inhomogeneously broadened absorption line can be used as a frequency-selectively addressed qubit. The proof of principle of the qubit-qubit interaction has been previously demonstrated. Thirdly, no special material engineering is required, and the crystal is commercially available. Ways of initializing a sub-ensemble of Pr ions as a qubit in the random system, manipulating the quantum state of the ions in a controlled way, and characterizing the quantum state created are presented. In order to achieve better scalability, the idea of letting a single rare-earth ion represent a qubit was investigated. The fidelity of the single-ion readout scheme was briefly studied. The influence of the energy transfer process between two neighbouring ions on quantum computing is discussed. A readout ion should possess a number of specific spectroscopic properties. Therefore, the position and the linewidths of the zero-phonon line of Ce ions were measured using an external cavity diode laser (at 371 nm) as the excitation source. The difference in the permanent dipole moment of the ground and excited states of Ce ions was measured in a photon echo experiment on Pr ions in a Ce-Pr co-doped Y2SiO5 crystal. The last and most important task was to realize single Ce ion detection. Fluorescence of Ce ions has been detected from a crystal, where there is on average 1 ion within 4.6 \micro m3 interacting with the excitation laser at a time. Estimates were made of the number of ions contributing to an observed signal. A trial experiment to investigate whether the signal was emitted by a single Ce ion was carried out, but was unsuccessful. Potential reasons why the experiment failed are presented.
Rare-earth ions doped into a transparent crystal can have optically excited states with coherence times of milliseconds and hyperfine levels with coherence times of hours when cooled down to liquid helium temperatures. This makes them attractive for developing quantum computing hardware. A quantum transistor can be implemented in a rare-earth-ion-doped crystal by utilizing a dipole blockade effect, where one excited ion prevents nearby ions from being excited. By using single rare-earth ions as qubits, the quantum processor is believed to be scalable to several qubits. In this thesis a readout mechanism for qubits represented by single ions (Eu or Pr) in a Y2SiO5 crystal is explored. A single cerium ion, in the same crystal as the qubits, could potentially be used as an indicator ion for non-demolition quantum state detection of the qubits. Cerium has a strong transition with high fluorescence yield which makes it possible to detect single ions. A cerium ion can be controlled by a qubit via the dipole blockade effect, and fluoresce if the qubit is in state |1> but stay dark if the qubit is in state |0>. Relevant spectroscopic properties of Ce:Y2SiO5 are studied, as well as interactions between cerium ions and qubit ions. The inhomogeneous and homogeneous linewidth of the Ce:Y2SiO5 4f-5d transition is measured and fluorescence spectra for ions in site 1 and site 2 are characterized. The change in electric dipole moment as a cerium ion is brought to the excited state is measured. The static dipole interaction between a single cerium ion and a qubit ion is shown to be strong enough for efficient qubit readout. Energy transfer from cerium to qubit ions is investigated. A lower bound on the cerium-qubit distance is found in order to avoid energy transfer. Satellite lines belonging to cerium-qubit pairs are mapped out. A microscope set-up is built to detect single ions in a crystal. Single ion detection is believed to be within reach.
In this work the inhomogeneous (zero-phonon line) and homogeneous linewidths and the permanent electric dipole moment change (averaged value of all dipole orientations) for the Ce 4f -5d transition in Y2SiO5 were measured in order to investigate the possibility for using Ce as a sensor to detect the hyperfine state of a spatially close-lying Pr or Eu ion. The experiments were carried out on Ce doped or Ce-Pr co-doped single Y2SiO5 crystals. The homogeneous linewidth is essentially limited by the excited state lifetime. Based on the
linewidth measurements, the oscillator strength, absorption cross section, and saturation intensity were calculated to be about 6.2(±1.7) × 10？7, 4.5(±1.3) × 10？19 m2, and 1.4(±0.4) × 107 W/m2, respectively. The difference
in permanent dipole moment, μCe, between the ground and excited states of the Ce ion was measured as 9.6(±5.3) × 10？30 C m. These measurements indicate that Ce is a promising readout ion to probe a single-ion qubit state for the quantum computing scheme using rare-earth ions.
In the last decade, the solid-state rare-earth-ion system has demonstrated increasing appeal for quantum computation. Despite this progress, two hardware limitations prevent a scalable implementation. These current limitations are the inability to miniaturise and the inability to perform single-ion qubit readout. This thesis addresses both these limitations and demonstrates that neither poses a fundamental restriction on increasing the scale of rare-earth-ion quantum computers. The challenge in miniaturising rare-earth-ion quantum hardware arises from the increases in homogeneous and inhomogeneous broadening that accompany micron-scale architectures. The success of miniaturised architectures, such as waveguides, depends on the properties of bulk ions being preserved within microns of the crystal surface. In addition, bulk ion properties must also be preserved in regions of high residual stress resultant from waveguide fabrication. The inhomogeneous and homogeneous properties of near-surface ions and ions in highly stressed environments in Pr3+:Y2SiO5 were studied via white light interferometry combined with micron resolution fluorescence microscopy. It was found that the bulk ion properties could be preserved both near the surface and in highly stressed regions close to micron-scale surface damage. The observation of excess inhomogeneous and homogeneous broadening was found to be consistent with the damage present at the crystal surface. The main outcome of the study was a set of waveguide fabrication guidelines to ensure that the appealing properties of bulk crystals can be maintained in a miniaturised architecture. The current inability to perform single-ion qubit readout is a consequence of the difficulty in isolating a single ion and lack of cyclicity in rare-earth-ion materials. Two techniques are proposed to form a solution: Stark activation and Zeeman enhanced cyclicity. When combined, these techniques offer direct readout for single-ion frequency-based quantum computing. Stark activation is designed to isolate a single rare-earth ion in a macroscopic crystal. The proposal is based on defining the condition for resonant excitation through a spatially varying electric field. A proof-of-principle experiment successfully created a 10 um absorption region within a millimetre thick crystal. In addition, the signal-to-noise ratio of the technique was characterised in experiments probing Pr3+:Y2SiO5 at the single-ion level. Future improvements to the apparatus should allow the nanometre spatial resolution and the noise level to be reduced to allow single-ion optical detection. High cyclicity is essential for high-fidelity optical readout of a single-ion qubit. Zeeman enhanced cyclicity achieves this by manipulating the hyperfine structure of the resonant crystal field levels to induce strong hyperfine selection rules. The technique is shown to be applicable to even the lowest symmetry sites. The simulated level of cyclicity in Pr3+:Y2SiO5 was greater than 99.99% by applying a 10 T field. The investigation of scalability in the rare-earth-ion system marks a movement away from the traditional ensemble-based methods in macroscopic crystals. This study required an understanding of these materials at a single-ion level and the development of high spatial resolution spectroscopic techniques. These advances extend the ability to engineer rare-earth-ion systems for applications including, but not limited to, quantum computing.
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.
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.
Quantum computing with single instances of rare earth-ions doped into inorganic crystals shows great promise as a scalable design in the field of quantum information. A detectable and controllable single readout ion is necessary for the scheme proposed in Lund to work. Due to its short excited state lifetime and its cyclable 4f-5d transition, cerium has been deemed suitable for just this purpose. The approach taken in Lund for this single cerium detection is to use a homemade confocal microscopy setup. In previous work using this setup on bulk crystals, it has been assumed that the undetectability of single cerium is due to out of focus ions contributing to a noise floor that is higher than the fluorescence signal from a single one. Hence single ion detection is being attempted in microcrystals. This thesis outlines the process behind converting the confocal microscope into a microcrystal detection setup. Subsequently, Ce3+:Y2SiO5 microcrystal spectroscopy experiments were performed. The energy level structure of cerium is reported to be identical to bulk, with a slight shift in wavelength, and the inhomogenous linewidth has proven to be inconclusive, although it hints towards being much wider than in bulk. Quantifying the homogenous linewidth of the cerium ions using Zeeman hole burning techniques was impervious to our attempts.