Modern experimental techniques can generate magnetic fields of the form H(t) = H0 z-hat + H1 [x-hat cos(ωt) + y-hat sin(ωt)], at frequencies within an order of magnitude of the nuclear magnetic resonance (NMR) and electron paramagnetic resonance (EPR) frequencies, ωn0 and ωe0, respectively, when acting on atoms or molecules. We derive simple closed-form expressions for the exact nuclear- and electronic-spin wave functions that enable controlled transitions between entangled states, allowing an atom or molecule to function as a quantum computer. These solutions also enable precise NMR or EPR measurements of nuclear moments in atoms and molecules. We present examples relevant to measurements of the nuclear moments of 14N, 7Li, and 133Cs. Because existing hyperfine measurements of the lowest three nuclear moments of 133Cs are mutually inconsistent, the proposed NMR/EPR experiments provide a route to measuring all seven of its nuclear moments with high precision.
Modern experimental techniques can generate magnetic fields of the form H(t) = H0 z-hat + H1 [x-hat cos(ωt) + y-hat sin(ωt)], at frequencies within an order of magnitude of the nuclear magnetic resonance (NMR) and electron paramagnetic resonance (EPR) frequencies, ωn0 and ωe0, respectively, when acting on atoms or molecules. We derive simple closed-form expressions for the exact nuclear- and electronic-spin wave functions that enable controlled transitions between entangled states, allowing an atom or molecule to function as a quantum computer. These solutions also enable precise NMR or EPR measurements of nuclear moments in atoms and molecules. We present examples relevant to measurements of the nuclear moments of 14N, 7Li, and 133Cs. Because existing hyperfine measurements of the lowest three nuclear moments of 133Cs are mutually inconsistent, the proposed NMR/EPR experiments provide a route to measuring all seven of its nuclear moments with high precision.
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.
In this work, we have been working on the concept of quantum entanglement. At first, we studied the theory of entanglement in its characterization and measurement, introducing a new scheme for detection of entanglement. The new approach links molecular-spin entities involving nuclear spins to quantum computing as more appropriate physical systems of interest. Then, we continued with the realization of entanglement in experiments. NMR has been the first choice due to its well approved advantages for quantum computing. NMR, however, has not been an appropriate system for demonstrating entangled states. Through a mathematical proof, NMR with low spin polarization has been invalidated for true implementations of non-local quantum algorithms, particularly supserdense coding. The point is that high spin polarization is inevitably required to acquire entanglement while in the current NMR it has been a formidable task to get highly polarized nuclear spins. In order to acquire high spin polarization, introducing electron spins can be much effective because of its three-order-of-magnitude larger gyromagnetic ratio compared to nuclear spins. Electron Nuclear DOuble Resonance (ENDOR) is spin manipulation technology that enables us to deal with both electron and nuclear spins. Thus, in this context, it can be more appropriate device for quantum computing. We emphasize that (pseudo)entanglement and interconversion between the entangled states have been realized with ENDOR on extremely stable organic molecular-spin entities. The required experimental conditions to obtain true quantum entanglement are also discussed. The appropriate entanglement witness for the corresponding ensemble quantum computing is introduced and examined.
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.
Nuclear Magnetic Resonance (NMR) forms a natural test-bed to perform quantum information processing (QIP) and has so far proven to be one of the most successful quantum information processors. The nuclear spins in a molecule treated as quantum bits or qubits which are the basic building blocks of a quantum computer. The development of NMR over half a century puts it in a platform where we can utilize its excellent control techniques over an ensemble of spin systems and perform quantum computation in a highly controlled way. Apart from a successful quantum information processor, NMR is also a highly powerful quantum platform where many of the potentially challenging quantum mechanical experiments can be performed.
The highly parallel nature of the fundamental principles of quantum mechanics means that certain key resource-intensive tasks --- including searching, code decryption and medical, chemical and material simulations --- can be computed polynomially or even exponentially faster with a quantum computer. In spite of its remarkably fast development, the field of quantum computing is still young, and a large-scale prototype using any one of the candidate quantum bits (or 'qubits') under investigation has yet to be developed. Spin-based qubits in condensed matter systems are excellent candidates. Spins controlled using magnetic resonance have provided the first, most advanced, and highest fidelity experimental demonstrations of quantum algorithms to date. Despite having highly promising control characteristics, most physical ensembles investigated using magnetic resonance are unable to produce entanglement, a critical missing ingredient for a pure-state quantum computer. Quantum objects are said to be entangled if they cannot be described individually: they remain fundamentally linked regardless of their physical separation. Such highly non-classical states can be exploited for a host of quantum technologies including teleportation, metrology, and quantum computation. Here I describe how to experimentally create, control and characterise entangled quantum ensembles using magnetic resonance. I first explore the relationship between entanglement and quantum metrology and demonstrate a sensitivity enhancement over classical resources using molecular sensors controlled with liquid-state nuclear magnetic resonance. I then examine the computational potential of irreversible relaxation processes in combination with traditional reversible magnetic resonance control techniques. I show how irreversible processes can polarise both nuclear and electronic spins, which improves the quality of qubit initialisation. I discuss the process of quantum state tomography, where an arbitrary quantum state can be accurately measured and characterised, including components which go undetected using traditional magnetic resonance techniques. Lastly, I combine the above findings to initialise, create and characterise entanglement between an ensemble of electron and nuclear spin defects in silicon. I further this by generating pseudo-entanglement between an ensemble of nuclear spins mediated by a transient electron spin in a molecular system. These findings help pave the way towards a particular architecture for a scalable, spin-based quantum computer.
Abstract Magnetic resonance methods and in particular Nuclear Magnetic Resonance in the liquid state were the first experimental techniques to implement quantum computing algorithms. The main drawbacks of these methods sofar have been the highly mixed nature of the quantum states and scalability issues. Recently, efforts have been made to address these problems by applying magnetic resonance to solid state systems at lower temperatures. In this contribution, we give an overview of our results on accurately controlling and measuring the quantum state of spin systems in the liquid and in particular in the solid state at low temperatures using Nuclear Magnetic Resonance and Electron Spin Resonance.