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 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.
Solid-state nuclear magnetic resonance (NMR) has emerged as an important technique for material characterization, finding extensive applications across a diverse range of disciplines including physics, materials science, chemistry, and biology. Its utility stems from the ability to probe the local atomic environments and molecular dynamics within solid materials, which provides information on the composition of the material. In recent years, the scope of solid-state NMR has expanded into the realm of quantum information science and technology, where its abundant many-body interactions pulse control methodologies make it have significant research value and application potential. This paper offers a comprehensive overview of the research objects and theoretical underpinnings of solid-state NMR, delving into the critical nuclear spin interaction mechanisms and their corresponding Hamiltonian forms. These interactions, which include dipolar coupling, chemical shift anisotropy, and quadrupolar interactions, are fundamental to the interpretation of NMR spectra and the understanding of material properties at the atomic level. Moreover, the paper introduces typical dynamical control methods employed in the manipulation of solid-state nuclear spins. Techniques such as dynamical decoupling, which mitigates the effects of spin-spin interactions to extend coherence times, and magic-angle spinning, which averages out anisotropic interactions to yield high-resolution spectra. These methods are essential for enhancing the sensitivity and resolution of NMR experiments, enabling the extraction of detailed structural and dynamic information from complex materials. Then we introduce some recent advancements in quantum control based on solid-state NMR, such as nuclear spin polarization enhancement techniques, which include dynamic nuclear polarization (DNP) and cross polarization (CP), significantly boost the sensitivity of NMR measurements. Additionally, the control techniques of Floquet average Hamiltonians are mentioned, showcasing their role in the precise manipulation of quantum states and the realization of quantum dynamics. Finally, the paper presents a series of seminal research works that illustrate the application of solid-state NMR quantum control technologies in the field of quantum simulation. These studies demonstrate how solid-state NMR can be leveraged to simulate and investigate quantum many-body systems, providing valuable insights into quantum phase transitions, entanglement dynamics, and other phenomena relevant to quantum information science. By bridging the gap between fundamental research and practical applications, solid-state NMR continues to play a crucial role in advancing our understanding of quantum materials and technologies.
Coupled electron-nuclear spins are promising physical systems for quantum in-formation processing: By combining the long coherence times of the nuclear spins with the ability to initialize, control, and measure the electron spin state, the favor-able properties of each spin species are utilized. This thesis discusses a procedure to initialize these nuclear spin qubits, and presents a vision of how these systems could be used as the fundamental processing unit of a quantum computer. The fo-cus of this thesis is on control of a system in which a single electron spin is coupled to N nuclear spins via resolvable anisotropic hyperfine (AHF) interactions. High-fidelity universal control of this le-Nn system is possible using only excitations on a single electron spin transition. This electron spin actuator control is implemented by using optimal control theory to find the modulation sequences that generate the desired unitary operations. Decoherence and the challenge of making useful qubits from these systems are also discussed. Experimental evidence of control using an electron spin actuator was acquired with a custom-built pulsed electron spin resonance spectrometer. Complex mod-
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.
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.
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.