Quantum computing set a goal to harness the quantum laws of physics and create \ncomputers more powerful than ever imagined. Different technologies can be chosen to implement quantum bits (qubits), each with their advantages and drawbacks. The idea of combining different technologies then seems natural in order to come up with an optimal quantum computer. \n \nIn this sense, Nuclear Magnetic Resonance (NMR) and Electron Spin Resonance (ESR) seem to be the perfect marriage. Indeed, while electron spins can perform quantum gates within nanoseconds, they have to fight very fast decoherence phenomena, the nuclear spins, on the other hand, require longer electromagnetic pulses to be rotated but can be controlled longer without loss of quantum information. Using electron spins as actuators and nuclear spins as memory then appears as the optimal use of this hybrid system. Another fact accounting for this association is that the control of the system through the electron spin requires techniques very similar to the well-known NMR ones. \n \nThis work focuses on characterizing as precisely as possible the Hamiltonian of a hybrid spin system in a solid-state single crystal, especially the electron-nuclear interactions, to perform high-fidelity control in a home-built pulsed ESR spectrometer. Using this knowledge, we show that we can choose the orientation of the magnetic field with respect to our crystal to obtain optimal experimental conditions. Indeed, with a good knowledge of the Hamiltonian of the system, we want demonstrate high-fidelity quantum control. \n \nThe final aim of this work is to dynamically supply highly polarized ancilla qubits that can be used in a Quantum Error Correction (QEC) experiment by implementing heat bath algorithmic cooling using a cold electron spin bath. This is an important step towards demonstrating the viability of spin systems for building quantum computers.
Quantum computing set a goal to harness the quantum laws of physics and create \ncomputers more powerful than ever imagined. Different technologies can be chosen to implement quantum bits (qubits), each with their advantages and drawbacks. The idea of combining different technologies then seems natural in order to come up with an optimal quantum computer. \n \nIn this sense, Nuclear Magnetic Resonance (NMR) and Electron Spin Resonance (ESR) seem to be the perfect marriage. Indeed, while electron spins can perform quantum gates within nanoseconds, they have to fight very fast decoherence phenomena, the nuclear spins, on the other hand, require longer electromagnetic pulses to be rotated but can be controlled longer without loss of quantum information. Using electron spins as actuators and nuclear spins as memory then appears as the optimal use of this hybrid system. Another fact accounting for this association is that the control of the system through the electron spin requires techniques very similar to the well-known NMR ones. \n \nThis work focuses on characterizing as precisely as possible the Hamiltonian of a hybrid spin system in a solid-state single crystal, especially the electron-nuclear interactions, to perform high-fidelity control in a home-built pulsed ESR spectrometer. Using this knowledge, we show that we can choose the orientation of the magnetic field with respect to our crystal to obtain optimal experimental conditions. Indeed, with a good knowledge of the Hamiltonian of the system, we want demonstrate high-fidelity quantum control. \n \nThe final aim of this work is to dynamically supply highly polarized ancilla qubits that can be used in a Quantum Error Correction (QEC) experiment by implementing heat bath algorithmic cooling using a cold electron spin bath. This is an important step towards demonstrating the viability of spin systems for building quantum computers.
The ability to perform quantum error correction (QEC) arbitrarily many cycles is a significant challenge for scalable quantum information processing (QIP). Key requirements for multiple-round QEC are a high degree of quantum control, the ability to efficiently characterize both intrinsic and extrinsic noise, and the ability to dynamically and efficiently extract entropy from ancilla qubits. Nuclear Magnetic Resonance (NMR) based quantum devices have demonstrated high control fidelity with up to 12 qubits, and the noise characterizations can be performed using an efficient protocol known as randomized benchmarking. One of the remaining challenges with NMR systems is that qubit initialization is normally only attainable via thermal equilibration. This results in very low polarizations in reasonable experimental conditions. Moving to electron-nuclear coupled spin systems in a single crystal is a promising solution to the ancilla qubit preparation problem. One obvious advantage of incorporating electron spins comes from higher gyromagnetic ratio of the electron which yields about three orders of magnitude larger thermal spin polarization than that of nuclear spins in the same experimental condition. In addition, fast control of nuclear spins is possible provided appropriate level of anisotropic hyperfine interaction strength. The nuclear spins can be polarized even beyond the thermal electron spin temperature using a technique Heat-Bath Algorithmic Cooling (HBAC). With theoretical ideas in hand, the next step is to develop classical instrumentations to control electron-nuclear coupled systems and accomplish high fidelity coherent control. Noise characterizations are also necessary for benchmarking the quality of control over the electron-nuclear spin system. \nI first present example applications of NMR QIP with small number of qubits: Testing a foundational question in quantum mechanics and measuring spectral density of noise in a quantum system. Then I report on our home-built X-band electron spin resonance (ESR) spectrometer and progress in achieving high fidelity coherent control of electron and nuclear spins for QIP. We focus on implementing nuclear spin manipulation via anisotropic hyperfine interaction and microwave (mw) control, but discussions also include electron nuclear double resonance (ENDOR) control techniques. We perform realistic algorithmic simulations to show that an experimental cooling of nuclear spins below electron thermal temperature is feasible, and to present the electron-nuclear spin systems as promising testbeds for scalable QIP.
ESR quantum computing presents faster means to perform gates on nuclear spins than the traditional NMR methods. This means ESR is a test-bed that can potentially be useful in ways that are not possible with NMR. The first step is to demonstrate universal control in the ESR system. This work focuses on spin systems with one electron spin and two nuclear spins. We try to demonstrate control over the nuclear spins using the electron as an actuator. \n \nIn order to perform the experiments, a customized ESR spectrometer was built in the lab. The main advantage of the home-built system is the ability to send arbitrary pulses to the spins. This ability is the key to perform high fidelity controls on the spin system. \n \nA customized low temperature probe was designed and built to have three features necessary for the experiments. First, it is possible to orient the sample, thus to change the spin Hamiltonian of the system, in situ. Second, the combined system is able to perform ESR experiments at liquid nitrogen and liquid helium temperatures and rotate the sample while it is cold. Last, the pulse bandwidth of the microwave resonator, which directly affects the fidelity of the gates, is held constant with respect to the sample temperature. \n \nSimulations of the experiments have been carried out and the results are promising. Preliminary experiments have been performed, the final set of experiments, demonstrating full quantum control of a three-spin system, are underway at present.
Standard CMOS circuits are expected to be no longer able to satisfy nowadays demand for higher performances and lower power consumption. This commits to look for new solutions. Quantum computation, whose fundamental quantity of information is the qubit, is a thoroughly new way of thinking to electronics. There are at least two main reasons for which quantum computing is expected to broaden computation horizons. First, specific algorithms can be engineered, manipulating the probability amplitudes of different states, to exploit the quantum superposition principle and achieve high parallelism. Second, it is expected to be spontaneously suitable to simulate complex quantum physical systems, as large molecules. Quantum computing requires the cooperation of several scientific fields. The leading idea has been to highlight the operations and algorithms a quantum computer must be able to perform and, then, to propose a hardware solution, providing the rigorous physical treatment mandatory for a deep understanding and for an appropriate modelling, something which is hard to find in nowadays literature. Thus, the first chapters address the quantum algorithms, focusing on Grover's search algorithm and deriving, from fundamentals, the corresponding circuit. The latter is then described in Quantum Assembly (QASM), which can be seen as the quantum equivalent of VHDL, and simulated on IBM Q Experience. The following chapters deal with a possible physical implementation of quantum processors: the encoding of qubits on nuclear spins in diamagnetic molecules. When a static magnetic field is applied to a spin-1/2 nucleus, two well-defined energy eigenstates arise, as a result of the Zeeman effect. Each of them can be associated with a qubit eigenstate. Thanks to nuclear magnetic resonance principles, the probability with which one of the two eigenstates is measured can be handled by the superposition of a radio frequency field at the resonance frequency of the nucleus. This can be interpreted as a rotation of the spin, and so of the qubit, about the RF field and enables the execution of single qubit quantum gates, since they are simple rotations of the state vector. The two-qubit CNOT gate is obtained through the interaction of spins via J-coupling. Considering that these gates constitute a universal set, every quantum algorithm can theoretically be run on an NMR processor. Different nuclei have different resonant frequencies, but the addressing of a specific spin can be achieved also in homonuclear molecules, since the resonant frequency depends also on the nuclear environment (nuclear shielding). While unwanted J-couplings can be removed thanks to refocusing, spin decoherence and relaxation phenomena force an upper limit to the allowed timescale. A main advantage of NMR is that this timescale is long, even at room temperature. Conversely, scalability is still an issue. A simple heteronuclear MATLAB model, based on the relations derived from first principles in the thesis, is proposed to prove the feasibility of NMR quantum processors. The input technological parameters, as chemical shielding and J-coupling, can be computed resorting on ORCA, or obtained from experimental data. The model, able to run a universal set of quantum gates and simple algorithms, can be useful to find an optimal operating point as a compromise between molecule physical properties and the quantities which can be controlled by nowadays NMR instrumentation.
Working on quantum systems entail different interests, for example, working on fundamental \nunderstanding of quantum systems also lay foundation for better quantum computation \ntechniques. A test for whether a system is behaving quantum mechanically or \nclassically is devised by Leggett and Garg in form of inequalities, called Leggett-Garg Inequalities \n(LGI). Such Inequalities are violated by a system whose evolution is governed \nby quantum mechanics. A precise experiment to violate LGIs require a guarantee that the \nmeasurement does not affect the system or its future dynamics. These Inequalities were \nproposed for dichotomic systems,systems which can have two outcomes. Here we present \nan LG experiment on a three-level quantum system, which theoretically have larger quantum \nupper bound than that of a two-level quantum system. This larger violation also \nprovides a bigger buffer to taking in account of the various experimental imperfections. \nPerforming a quantum computing task requires precise level of control to initialize, \nperform and measure the quantum system. With increasing size of the quantum processor \nthe challenge is to maintain optimal control. Nuclear Magnetic Resonance (NMR) has \nalways been a very faithful test-bed for quantum processing ideas. In NMR, we perform \nRadio Frequency (RF) pulses to control and steer the system to the desired state. Most \nused method to derive the exact frequency and amplitude of these pulses for a given \ntask is based on gradient. Although systematic, one have to simulate these pulses on \na classical computer first, which makes the task very inefficient. We report a a way of \nperforming optimization with a hybrid quantum-classical scheme. This scheme helps us \nperform classically harder computational tasks on the quantum processor. We optimize \npulses which drive our system from 7-coherence state to 12-coherence state on a 12-qubit \nNMR processor. \nElectron Spin Resonance (ESR) employs the same techniques as of NMR but having \nadvantage in larger polarization compared to later. Although this does not imply better \ncontrol, cause the frequency at which pulses are required to control an ESR system fall into \nmicrowave region. Microwave frequency are harder to control electronically, thus making \nit harder for performing ESR quantum computing. The hybrid scheme used in NMR \nexperiment relies on some ideal pulses which are needed to be optimized classically. We \nalleviate this requirement by using finite difference method of calculating gradient. We \ncompare these methods with the earlier methods to show the superiority of such a scheme. \nState-to-state transfer pulses are sufficient for most of the quantum computing task, \nbut, an universal quantum information implementation requires state independent pulses. \nThe techniques used in optimizing state-to-state pulses can be modified to optimize for a \nstate independent pulse. We show that this methods scale polynomially with the number \nof qubits and is general in terms of its implementation. We further reduce the resource \nrequirement by using a NMR related implementation.
The goal of this project was to improve our control over nuclear spins in the solid state, and to extend this control to coupled electron-nuclear spins. Our key results are summarized below. 1. We extended the control techniques developed in liquid state NMR quantum information processing to the control of a three-qubit solid state NMR quantum information processor. 2. To explore multi-body spin dynamics and their sensitivity to decoherence, we have measured the decay of NMR multiple quantum coherence intensities in the presence and absence of the dipolar Hamiltonian, in a cubic and a one-dimensional spin system. 3. We also studied the transport of polarization in the one-dimensional fluoroapatite system, both experimentally and theoretically, and created special states in which the polarization is localized to the ends of the chain. This enables both universal Quantum Computing and Quantum Simulation in 1-D systems. 4. We devised a novel scheme for electron-nuclear quantum information processing that exploits the anisotropic hyperfine coupling. This scheme enables universal control over a 1-electron, N-nuclear spin system, addressing only a single electron spin transition. Not having to address the nuclear spins directly significantly speeds up the control. We designed and fabricated a pulsed electron spin resonance spectrometer, along with a cryogenic probe which we used to experimentally implement this scheme on a single crystal sample of irradiated malonic acid. 5. We demonstrated the role of nuclear spin dipolar diffusion in dynamic nuclear polarization (DNP) experiments, in dielectric samples with abundant nuclear spins. We achieved a 29Si polarization of 8.3% at 66 GHz and 1.1 K in single crystal P-doped, the highest ever reported, using DNP.
The subject of this thesis are experimental procedures for preparation, manipulation, and detection of specific quantum states of spin systems in the context of quantum computing. Nuclear magnetic resonance (NMR) and electron spin resonance (ESR) methods were used. The systems studied were small molecules in liquid state, small molecules embedded in a liquid crystal matrix, and paramagnetic centers in single crystals. The nuclear 19F spins of 2,3,4-Trifluoroaniline were used as qubits to implement the three-qubit Deutsch-Josza algorithm using high-resolution NMR. A classification of the Deutsch-Josza functions according to the operator representation of the corresponding oracle transformations was given. Different classes of functions may produce full, partial or no entanglement in the output states of the algorithm. This entanglement content is not immediately evident from the output states themselves. A procedure was given for mapping of the output states onto Bell- or GHZ-states by means of local transformations which preserve the entanglement content. A method for the visualization of single-spin unitary transformations was also presented. This visual representation can facilitate analysis and design of shaped rf pulses. For the purpose of quantum computing, it can be useful to suppress couplings between qubits during the application of finite-length single-qubit gates. The feasibility of this idea was demonstrated using small molecules in a liquid crystal matrix. In a series of proof-of-principle experiments, it was shown that the magic-echo sequence can be used to suppress the dipole-dipole coupling between spins and simultaneously selectively address a single spin by a soft rf pulse. The S-bus concept for spin-quantum computing holds some scalability promise and provides a testbed for studies of large, strongly coupled quantum registers. Single-crystal CaF2 weakly doped with Ce was used to implement the concept. The nine 19F nuclear spins adjacent to the paramagnetic Ce-ion serve as qubits while the electron spin plays the role of a quantum bus. The S-bus theory was tested experimentally. Procedures were given for the measurement of parameters characterizing the quantum state of the nuclear spins. An exact numeric treatment of this ten-spin system was done to aid in understanding the experimental findings. For a pair of nuclear spins with negligible direct dipolar coupling, the CNOT operation was implemented. The spin-spin coupling mediated by the bus spin was utilized for that purpose. The four Bell-states of these two distant spins were created. An experiment was performed who's signature allows those four entangled states to be distinguished. The paramagnetic cluster in CaF2:Ce is embedded in an extended network of 19F nuclear spins. This network is a powerful source of decoherence. A number of existing and a newly designed pulse sequence were tested with respect to their ability to suppress decoherence and their aptitude for use in quantum computing.