Donors in silicon, which combine an electron and nuclear spin, are some of the most promising candidates for quantum information. The electron spin has been proposed as a register with fast manipulation and the nuclear spin as a memory with long coherence times. However, this division reduces the complexity of the donor system, in particular behaviors emerging from their interaction. In natural silicon, there is also the presence of 29Si nuclear spins in the donor environment; though they are generally seen as a source of decoherence, they are quantum systems that can be investigated too. The main subject of this thesis is the study of the interactions between these various spins, using different methods to probe and control them. I first concentrate on the coupling between the donor and the 29Si spins. This coupling can be perturbed by the application of dynamical decoupling on the donor electron spin, whose evolution can be made sensitive to the number of 29Si spins interacting together. I then propose an error correction scheme using the donor and 29Si spins, showing key requirements such as coherence times and methods for manipulation and initialization. Secondly, I focus on the donor itself, in a regime where the hyperfine and Zeeman couplings compete with each other. Here, the spin transitions can have different sensitivities to the magnetic environment, and can even be suppressed to first order, resulting in coherence times up to seconds with electron spin-like manipulation times. Controlling this sensitivity was also used to probe the effect of the donor on the 29Si spin bath evolution. Finally, I use electric fields to modulate the hyperfine coupling within the donor. I first characterize the spins’ sensitivity to the electric field, and then demonstrate electrical switching of the nuclear spin response to an external magnetic excitation.
Donors in silicon, which combine an electron and nuclear spin, are some of the most promising candidates for quantum information. The electron spin has been proposed as a register with fast manipulation and the nuclear spin as a memory with long coherence times. However, this division reduces the complexity of the donor system, in particular behaviors emerging from their interaction. In natural silicon, there is also the presence of 29Si nuclear spins in the donor environment; though they are generally seen as a source of decoherence, they are quantum systems that can be investigated too. The main subject of this thesis is the study of the interactions between these various spins, using different methods to probe and control them. I first concentrate on the coupling between the donor and the 29Si spins. This coupling can be perturbed by the application of dynamical decoupling on the donor electron spin, whose evolution can be made sensitive to the number of 29Si spins interacting together. I then propose an error correction scheme using the donor and 29Si spins, showing key requirements such as coherence times and methods for manipulation and initialization. Secondly, I focus on the donor itself, in a regime where the hyperfine and Zeeman couplings compete with each other. Here, the spin transitions can have different sensitivities to the magnetic environment, and can even be suppressed to first order, resulting in coherence times up to seconds with electron spin-like manipulation times. Controlling this sensitivity was also used to probe the effect of the donor on the 29Si spin bath evolution. Finally, I use electric fields to modulate the hyperfine coupling within the donor. I first characterize the spins’ sensitivity to the electric field, and then demonstrate electrical switching of the nuclear spin response to an external magnetic excitation.
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.
Spins in nuclear-spin-free solid state systems such as isotopically purified 28Si have seen extensive research as candidates for quantum information storage and processing, thanks to their long spin coherence lifetimes [1]. Strongly coupling such spins to a high Q superconducting resonator provides a route to develop microwave quantum memories. Bismuth donor spins can be tuned to so-called ‘clock transitions’, which, due to their insensitivity to magnetic field noise, can have electron spin coherence times as long as 3 seconds [2]. The system also possesses ‘hyperfine clock transitions’, which are insensitive to changes in the hyperfine coupling constant, and which may mitigate the effects of strain on the transition. Achieving coupling to such transitions requires resonators which are both magnetic-field resilient, and frequency tuneable. This thesis outlines the work done towards realising a quantum memory using Bi donors in silicon, from resonator design and fabrication, coupling these to implanted Bi spins in silicon and tuning to various clock transitions, through to storage and retrieval of few-photon excitations in a spin ensemble and their retrieval over 100 ms later.
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.
Electric fields can be used to tune donor spins in silicon using the Stark shift, whereby the donor electron wave function is displaced by an electric field, modifying the hyperfine coupling between the electron spin and the donor nuclear spin. We present a technique based on dynamic decoupling of the electron spin to accurately determine the Stark shift, and illustrate this using antimony donors in isotopically purified silicon-28. We then demonstrate two different methods to use a dc electric field combined with an applied resonant radio-frequency (rf) field to conditionally control donor nuclear spins. The first method combines an electric-field induced conditional phase gate with standard rf pulses, and the second one simply detunes the spins off resonance. Finally, we consider different strategies to reduce the effect of electric field inhomogeneities and obtain above 90% process fidelities.
This dissertation is a study of the decoherence of a solid-state spin qubit, either that of a localized electron spin or a donor nucleus, caused by a nuclear spin bath relevant to semiconductor quantum computer architectures. In the presence of an external magnetic field and at low temperatures, the dominant decoherence mechanism is the spectral diffusion of the qubit spin resonance frequency due to the temporally fluctuating random magnetic field associated with the dipolar interaction induced flip-flops of nuclear spin pairs. The qubit spin dephasing due to this random magnetic field depends intricately on the quantum dynamics of the nuclear spin bath, making the coupled decoherence problem difficult to solve. We provide a formally exact solution of this non-Markovian quantum decoherence problem which numerically calculates accurate spin decoherence at short times, of particular relevance in solid-state spin quantum computer architectures. A quantum cluster expansion method is motivated, developed, and tested for the spectral diffusion problem. The method is applicable to any ideal pulse sequence applied to the qubit. Dynamical decoupling sequences, which aim to prolong qubit coherence, are analyzed. In particular, concatenated dynamical decoupling sequences are shown to prolong not only the coherence time over the entire sequence but also the length of time between pulses necessary to maintain coherence. This is shown to result from successive low-order cancellations in applicable perturbative expansions with each level of concatenation. Each cancellation, however, will require the inclusion, in the cluster expansion, of increasingly large clusters to obtain the lowest-order results. These larger clusters in the lowest order often dominate decoherence and therefore invalidate, as being overly optimistic, the pair approximation as a means to study the effect of concatenated dynamical decoupling. We present numerical results from our cluster expansion technique for echoes of single (Hahn), concatenated, and periodic pulse sequences using realistic models of a localized electron in phosphorus doped Si and in a GaAs quantum dot and of a P donor nucleus in Si or GaAs. In the Si:P electron spin decoherence problem, we consider, along with spectral diffusion, the effects of anisotropic hyperfine (AHF) interactions and suggest a technique to suppress electron spin echo envelope modulations (ESEEM), an additional source of decoherence resulting from the AHF interactions. Our calculations for the Si:P Hahn echoes, including the effects of both anisotropic hyperfine interactions and spectral diffusion, are in excellent agreement with experimental results. Our calculations of concatenated pulse sequence echoes offer important predictions for the effectiveness of a promising strategy to preserve qubit coherence in semiconductor quantum computer architectures.
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.