Conventional computing faces a huge technical challenge as traditional transistors will soon reach their size limitations. This will halt progress in reaching faster processing speeds and to overcome this problem, require an entirely new approach. Quantum computing (QC) is a natural solution offering a route to miniaturisation by, for example, storing information in electron or nuclear spin states, whilst harnessing the power of quantum physics to perform certain calculations exponentially faster than its classical counterpart. However, QCs face many difficulties, such as, protecting the quantum-bit (qubit) from the environment and its irreversible loss through the process of decoherence.Hybrid systems provide a route to harnessing the benefits of multiple degrees of freedom through the coherent transfer of quantum information between them. In this thesis I show coherent qubit transfer between electron and nuclear spin states in a 15N@C60 molecular system (comprising a nitrogen atom encapsulated in a carbon cage) and a solid state system, using phosphorous donors in silicon (Si:P). The propagation uses a series of resonant mi- crowave and radiofrequency pulses and is shown with a two-way fidelity of around 90% for an arbitrary qubit state. The transfer allows quantum information to be held in the nuclear spin for up to 3 orders of magnitude longer than in the electron spin, producing a 15N@C60 and Si:P ‘quantum memory’ of up to 130 ms and 1.75 s, respectively. I show electron and nuclear spin relaxation (T1), in both systems, is dominated by a two-phonon process resonant with an excited state, with a constant electron/nuclear T1 ratio. The thesis further investigates the decoherence and relaxation properties of metal atoms encapsulated in a carbon cage, termed metallofullerenes, discovering that exceptionally long electron spin decoherence times are possible, such that these can be considered a viable QC candidate.
Conventional computing faces a huge technical challenge as traditional transistors will soon reach their size limitations. This will halt progress in reaching faster processing speeds and to overcome this problem, require an entirely new approach. Quantum computing (QC) is a natural solution offering a route to miniaturisation by, for example, storing information in electron or nuclear spin states, whilst harnessing the power of quantum physics to perform certain calculations exponentially faster than its classical counterpart. However, QCs face many difficulties, such as, protecting the quantum-bit (qubit) from the environment and its irreversible loss through the process of decoherence.Hybrid systems provide a route to harnessing the benefits of multiple degrees of freedom through the coherent transfer of quantum information between them. In this thesis I show coherent qubit transfer between electron and nuclear spin states in a 15N@C60 molecular system (comprising a nitrogen atom encapsulated in a carbon cage) and a solid state system, using phosphorous donors in silicon (Si:P). The propagation uses a series of resonant mi- crowave and radiofrequency pulses and is shown with a two-way fidelity of around 90% for an arbitrary qubit state. The transfer allows quantum information to be held in the nuclear spin for up to 3 orders of magnitude longer than in the electron spin, producing a 15N@C60 and Si:P ‘quantum memory’ of up to 130 ms and 1.75 s, respectively. I show electron and nuclear spin relaxation (T1), in both systems, is dominated by a two-phonon process resonant with an excited state, with a constant electron/nuclear T1 ratio. The thesis further investigates the decoherence and relaxation properties of metal atoms encapsulated in a carbon cage, termed metallofullerenes, discovering that exceptionally long electron spin decoherence times are possible, such that these can be considered a viable QC candidate.
Quantum physics governs the world at the microscopic scale and determines the properties of matter. While classical computers exploit quantum phenomena passively by relying on transistor technology, the concept of a quantum computer with active control over quantum states promises unprecedented possibilities for information encoding and processing. Already developed quantum algorithms are known to perform certain tasks faster than any existing classical algorithms, and quantum computers also promise the possibility for precise simulations of complex quantum systems, a task infeasible for classical computers. These points emphasize the need for the development of quantum computers. Considering quantum computers, the fundamental unit of information is a qubit, a two-level quantum system. Qubits, in contrast to classical bits which are either in state 0 or 1, can exist in quantum superposition of the states 0 and 1, allowing for more complex and parallel computations. While there are many options to encode a logical qubit in a physical system, spin 1/2 particles are considered a natural choice because their spin degree of freedom defines a qubit intrinsically. Semiconductors are a promising platform for hosting spin qubits, as they enable the confinement of electrons with spin 1/2 either through gate-defined quantum dots (QDs) or donor atoms. Among the possible choices of donor atoms, phosphorous 31P is particularly noteworthy because its nucleus has nuclear spin 1/2. Nuclear spins are prime candidates for qubit implementation because they demonstrated exceptionally long coherence times, but the underlying good isolation from their environment is a challenge when it comes to readout and control. In this thesis, we face this challenge by proposing a hybrid quantum dot-donor (QDD) system consisting of a gate defined silicon (Si) QD and a thereto laterally displaced 31P phosphorous donor atom implanted in the Si host material. A single electron is presumed to be confined in the system, which can be moved between the QD and the donor on demand. If its wave function overlaps with the donor atom, electron spin and the donor nuclear spin interact via the hyperfine interaction and the electron can act as a mediator between the nuclear spin qubit and the environment for readout and control, whereas the nuclear spin qubit can be set in an idling mode by shifting the electron to the QD. Importantly, the proposed system can be embedded in circuit quantum electrodynamics (cQED) architectures enabling strong coupling between the system’s electron spin and microwave resonator photons. This coupling is fundamental for the research presented in this thesis. Analyzing the envisioned system, we first propose a novel method for nuclear-spin readout by probing the resonator transmission. This method is based on the observation that the signature of strong electron spin-photon coupling in the resonator transmission is altered due to the hyperfine interaction, in such a manner that well separated signatures for the electron spin-photon coupling conditioned on the state of the nuclear spin arise. As the next step, we turn our attention to the control of nuclear spin qubits and especially to the challenge of realizing a two-qubit gate between distant nuclear spins. In this course, we derive an effective nuclear spin-photon coupling. While expected to be weak, this interaction can be harnessed to couple the nuclear spins of two distant QDD systems dispersively to a microwave resonator resulting in an entangling nuclear spin two-qubit √iSWAP gate with a gate fidelity approaching 90%. These two key findings represent a significant and valuable contribution to the field of quantum information processing using nuclear spins.
A major problem facing the realisation of scalable solid-state quantum computing is that of overcoming decoherence - the process whereby phase information encoded in a qubit is lost as the qubit interacts with its environment. Due to the vast number of environmental degrees of freedom, it is challenging to accurately calculate decoherence times T2, especially when the qubit and environment are highly correlated. Hybrid or mixed electron-nuclear spin qubits, such as donors in silicon, possess 'optimal working points' (OWPs) which are sweet-spots for reduced decoherence in magnetic fields. Analysis of sharp variations of T2 near OWPs was previously based on insensitivity to classical noise, even though hybrid qubits are situated in highly correlated quantum environments, such as the nuclear spin bath of 29Si impurities. This presented limited understanding of the decoherence mechanism and gave unreliable predictions for T2. I present quantum many-body calculations of the qubit-bath dynamics, which (i) yield T2 for hybrid qubits in excellent agreement with experiments in multiple regimes, (ii) elucidate the many-body nature of the nuclear spin bath and (iii) expose significant differences between quantum-bath and classical-field decoherence. To achieve these, the cluster correlation expansion was adapted to include electron-nuclear state mixing. In addition, an analysis supported by experiment was carried out to characterise the nuclear spin bath for a bismuth donor as the hybrid qubit, a simple analytical formula for T2 was derived with predictions in agreement with experiment, and the established method of dynamical decoupling was combined with operating near OWPs in order to maximise T2. Finally, the decoherence of a 29Si spin in proximity to the hybrid qubit was studied, in order to establish the feasibility for its use as a quantum register.
Spin is a quantum mechanical property that describes the magnetic orientation of elementary and composite particles such as electrons and nuclei. For spin-half particles placed in a magnetic field, two states with differing energies are defined. Proposals exist for developing a revolutionary kind of computer that encodes bits of information on the states of a simple quantum two-level system - like those of a spin in a magnetic field. These quantum computers exploit the fundamental principles of quantum mechanics in order to perform certain calculations exponentially faster than their classical counterparts. Key to the development of such a device is the identification of potential systems that are suitable for employment as a quantum bit (qubit). This thesis explores quantum bits constructed from the spin states of single atoms hosted in silicon semiconductor devices. Silicon is an exceptional platform for spin-based quantum computing - in addition to being the dominant material in the microelectronic industry, it is also predominantly composed of nuclear spin-zero isotopes, providing very little background magnetic disturbance. The donor-atom phosphorus (31P) is investigated here. It possesses a nucleus that binds an additional electron to its positive charge, providing two distinct spin qubits. Here, several world-first experimental milestones in spin-based quantum information processing are reported. First, the readout of the electron spin is demonstrated in single-shot, using a silicon device which combines implanted phosphorus donors with a sensitive nanoscale electrometer. Then, the electron spin is coherently operated as a qubit by delivering on-chip microwave excitations. Combining the electron spin detection and control capabilities enables a quantum non-demolition measurement of the single 31P nuclear spin. Experiments yield exceptional nuclear readout fidelities - the highest for any solid-state qubit. Through an application of nuclear magnetic resonance, high-fidelity quantum control of the nuclear spin qubit is demonstrated. Finally, a single spin-bearing silicon nucleus (29Si) coupled to the electron spin is detected in single-shot and operated as a qubit. These results, along with the clear pathways identified for improving device performance, illustrate that single-atom electron and nuclear spin qubits in silicon constitute an excellent basis on which to construct a quantum computer.
Abstract Long coherence times and fast gate operations are desirable but often conflicting requirements for physical qubits. This conflict can be resolved by resorting to fast qubits for operations, and by storing their state in a ‘quantum memory’ while idle. The 31 P donor in silicon comes naturally equipped with a fast qubit (the electron spin) and a long-lived qubit (the 31 P nuclear spin), coexisting in a bound state at cryogenic temperatures. Here, we demonstrate storage and retrieval of quantum information from a single donor electron spin to its host phosphorus nucleus in isotopically enriched 28 Si. The fidelity of the memory process is characterised via both state and process tomography. We report an overall process fidelity F p ≈ 81 %, and memory storage times up to 80 ms. These values are limited by a transient shift of the electron spin resonance frequency following high-power radiofrequency pulses.
Nuclear spin registers in the vicinity of electron spins in solid state systems offer a powerful resource to address the challenge of scalability in quantum architectures. We investigate here the properties of 29 Si nuclear spins surrounding donor atoms in silicon, and consider the use of such spins, combined with the donor nuclear spin, as a quantum register coupled to the donor electron spin. We find the coherence of the nearby 29 Si nuclear spins is effectively protected by the presence of the donor electron spin, leading to coherence times in the second timescale—over two orders of magnitude greater than the coherence times in bulk silicon. We theoretically investigate the use of such a register for quantum error correction (QEC), including methods to protect nuclear spins from the ionisation/neutralisation of the donor, which is necessary for the re-initialisation of the ancillae qubits. This provides a route for multi-round QEC using donors in silicon.