Hardware of modern quantum computing (QC) platforms is based mainly on superconductors and ion traps. It demands ultra-low temperature and high vacuum. Practicality and scaling up thus remain questionable. This work analyzes the alternative based on the micro- and nanoparticles of the compounds of Rare Earth (RE) elements, such as phosphors NaYF4: X3+ (X stands for Tm, Er, etc.), embedded in polymer matrices. The qubits in these systems correspond to the quantum levels of 4f electrons of RE ions, and they have optical frequencies. Qubit formation is supported by the properties of RE ions: (a) weak interaction with the environment, (b) strong inhomogeneous crystal field, and (c) the ability of neighboring ions, being in some 4f states, to interact with each other through the mechanism of Stark blockade. The latter is required for quantum conditional gate operations, such as Controlled NOT (CNOT – the basic block of a quantum computer circuit). Optical spectroscopy indicated that CNOT gate can be implemented, for instance, using the transitions in for-level system of Tm3+ ions |3H6> (ground state), |3H4> (state 0), |1D2> (state 1), and |1I6> (auxiliary state 1’) activated with conventional tunable lasers at 451, 653, 798, and 1459 nm. We also considered the PT- and anti-PT-symmetry on the decoherence rate of the qubits. PT-symmetric Hamiltonian H(x) has its real part symmetric versus x-coordinate, and the anti-PT-symmetric one is anti-symmetric. Anti-PT symmetric qubits tend to be more decoherence stable than the others. It was suggested that the anti-PT-symmetry can be introduce via coupling of the qubits to anti-PT-symmetric cavities using RE-doped compounds as gain media.
Hardware of modern quantum computing (QC) platforms is based mainly on superconductors and ion traps. It demands ultra-low temperature and high vacuum. Practicality and scaling up thus remain questionable. This work analyzes the alternative based on the micro- and nanoparticles of the compounds of Rare Earth (RE) elements, such as phosphors NaYF4: X3+ (X stands for Tm, Er, etc.), embedded in polymer matrices. The qubits in these systems correspond to the quantum levels of 4f electrons of RE ions, and they have optical frequencies. Qubit formation is supported by the properties of RE ions: (a) weak interaction with the environment, (b) strong inhomogeneous crystal field, and (c) the ability of neighboring ions, being in some 4f states, to interact with each other through the mechanism of Stark blockade. The latter is required for quantum conditional gate operations, such as Controlled NOT (CNOT – the basic block of a quantum computer circuit). Optical spectroscopy indicated that CNOT gate can be implemented, for instance, using the transitions in for-level system of Tm3+ ions |3H6> (ground state), |3H4> (state 0), |1D2> (state 1), and |1I6> (auxiliary state 1’) activated with conventional tunable lasers at 451, 653, 798, and 1459 nm. We also considered the PT- and anti-PT-symmetry on the decoherence rate of the qubits. PT-symmetric Hamiltonian H(x) has its real part symmetric versus x-coordinate, and the anti-PT-symmetric one is anti-symmetric. Anti-PT symmetric qubits tend to be more decoherence stable than the others. It was suggested that the anti-PT-symmetry can be introduce via coupling of the qubits to anti-PT-symmetric cavities using RE-doped compounds as gain media.
Several platforms are being considered as hardware for quantum technologies. For quantum computing (QC), superconducting qubits and artificially trapped ions are among the leading platforms, but many others also show promise, e.g. photons, cold atoms, defect centers including Rare-Earth (RE) ions. So far, results are limited to the regime of noisy intermediate scale qubits (NISQ), with a small number of qubits and a limited connectivity, and it is likely that future QC hardware will utilize several existing platforms in different ways. Thus, it currently makes sense to invest resources broadly and explore the full range of promising routes to quantum technology. Rare-earth ions in solids constitute one of the most versatile platforms for future quantum technology. One advantage is good coherence properties even when confined in strong natural traps inside a solid-state matrix. This confinement allows very high qubit densities and correspondingly strong ion-ion couplings. In addition, although their fluorescence is generally weak, cavity integration can enhance the emission greatly and enable very good connections to photonic circuits, including at the telecom wavelengths, making them promising systems for long-term scalability. The primary aim of this roadmap is to provide a complete picture of what components a RE quantum computer would consist of, to describe the details of all parts required to achieve a scalable system, and to discuss the most promising paths to reach it. In brief, we find that clusters of 50-100 single RE ions can act as high fidelity qubits in small processors, occupying only about (10 nm)^3. Due to the high capacity for integration of the RE systems, they be optically read out and connected to other such clusters for larger scalability. We make suggestions for future improvements, which could allow the REQC platform to be a leading one.
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.
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.
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 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.
Rare-earth-ion doped crystals are an interesting system for quantum computing investigations due to their long optical and hyperfine coherence times. In particular, the ground-state coherence times can be longer than one second, which makes them perfect for long-term storage of quantum states. They also have the advantage of being a solid-state system. At present, many of the fundamental requirements for quantum computing have been demonstrated using rare-earth-ions; however, quantum state readout has yet to be achieved. The strong-coupling regime is of great importance in cavity quantum electrodynamics, as in this regime interactions between single atoms and single photons can be realized. Strong coupling thereby provides a method of enabling qubit-qubit interactions. It is desirable to achieve this regime with rare-earth-ion doped resonators, as it would enable on-demand readout of quantum states, a necessity for quantum computing, and provide the scalability required for implementation of quantum networks. This thesis describes the work that has gone into investigating the suitability of rare-earth-ion doped whispering-gallery mode resonators for quantum computing applications. A theoretical analysis of the strong-coupling regime is performed, followed by experiments investigating the properties of ions in resonators, and of new rare-earth-ion materials. A final set of experiments studies a new quantum memory protocol for use with rare-earth-ions. A theoretical investigation is undertaken to determine whether the strong-coupling regime will be attainable with rare-earth-ion doped whispering-gallery mode resonators. Emphasis is given to determining which rare-earth-ion materials will have the best properties when used as resonators. Specific applications of the strong-coupling regime are examined for this system; in particular, whether it will be possible to demonstrate the reversible transfer of quantum states, and detection of single dopants. Experiments are performed, measuring the properties of millimetre-sized Pr3+:Y2SiO5 resonators. Direct measurements of cavity quantum electrodynamics parameters are made using photon echoes, giving good agreement with theoretical predictions. Interactions between the atom and cavity are observed and a theoretical model is presented to describe these effects. Thus, a more realistic picture is obtained of the experimental requirements for achieving the strong-coupling regime. The properties of different rare-earth-ion doped materials are measured and analysed to determine their suitability for quantum computing applications. The spin Hamiltonian parameters of Pr3+:YAG are measured using Raman heterodyne spectroscopy, and then used to find the optical transitions with zero first-order Zeeman shift, as this should allow the coherence time to be extended to a point where this system is useful for resonator applications. Hyperfine transitions with zero first-order Zeeman shift are also calculated for Er3+:Y2SiO5, with the aim of enabling long-term storage in a telecommunication-wavelength memory. The thesis concludes with an experimental investigation into a new quantum memory technique that does not require spectral hole burning. The hybrid photon echo rephasing protocol uses strong optical pulses to perform rephasing, thus utilizing the advantageous properties of the two-pulse photon echo. Furthermore, the use of external broadening fields removes the usual problem of noise from amplified spontaneous emission. The properties of this memory are examined using a Pr3+:Y2SiO5 crystal.