This thesis is concerned with the control of quantum systems.Given a Hamiltonian model of a quantum system, we are interested in finding controls-typically shaped electromagnetic pulses-that steer the evolution of the system toward a desired target operation.For this we employ a numerical optimisation method known as the GRAPE algorithm.For particular experimental systems, we design control schemes that respect constraints of robustness and addressability, and are within the reach of the experimental hardware.A general procedure is given for specifying a Hamiltonian model of a driven N -level system and converting it to an appropriate rotating frame.This is then applied together with the numerical algorithm to design improved schemes for two different systems, where laser fields manipulate orbital and hyperfine states of Pr 3+ and Rb.The generation of cluster states in Ising-coupled systems is also studied.We find that, in the ideal case, the solution of evolving only under the coupling Hamiltonian is not time-optimal.This surprising result is in contrast to the known cases for unitary gates.For a symmetrised three-qubit example, we provide a geometrical interpretation of this.Numerically optimised control schemes are then developed for a nonideal coupling topology, modelling an experimental configuration of trapped ions.Controls for the implementation of the two-qubit Deutsch and Grover algorithms are designed for a pair of 13 C nuclear spins at a nitrogen vacancy center in diamond.These implementations are robust to experimental errors, and found to be reproduced with high accuracy on a VFG-150 pulse generator.We also consider two-qubit gate synthesis in a system of superconducting qubits coupled by mii xii CONTENTS C.4 Examples of time-optimal gates . . . . . . . .
This thesis is concerned with the control of quantum systems.Given a Hamiltonian model of a quantum system, we are interested in finding controls-typically shaped electromagnetic pulses-that steer the evolution of the system toward a desired target operation.For this we employ a numerical optimisation method known as the GRAPE algorithm.For particular experimental systems, we design control schemes that respect constraints of robustness and addressability, and are within the reach of the experimental hardware.A general procedure is given for specifying a Hamiltonian model of a driven N -level system and converting it to an appropriate rotating frame.This is then applied together with the numerical algorithm to design improved schemes for two different systems, where laser fields manipulate orbital and hyperfine states of Pr 3+ and Rb.The generation of cluster states in Ising-coupled systems is also studied.We find that, in the ideal case, the solution of evolving only under the coupling Hamiltonian is not time-optimal.This surprising result is in contrast to the known cases for unitary gates.For a symmetrised three-qubit example, we provide a geometrical interpretation of this.Numerically optimised control schemes are then developed for a nonideal coupling topology, modelling an experimental configuration of trapped ions.Controls for the implementation of the two-qubit Deutsch and Grover algorithms are designed for a pair of 13 C nuclear spins at a nitrogen vacancy center in diamond.These implementations are robust to experimental errors, and found to be reproduced with high accuracy on a VFG-150 pulse generator.We also consider two-qubit gate synthesis in a system of superconducting qubits coupled by mii xii CONTENTS C.4 Examples of time-optimal gates . . . . . . . .
An exquisite control over the dynamics of a quantum system is essential for realizing any quantum technology. This thesis presents some practical and efficient strategies for coherent quantum control: a paradigm for controlling quantum dynamics using electromagnetic fields. Coherent control is a common framework for describing the physical implementation of quantum logic gates in several quantum information processing platforms including superconducting qubits and trapped ions. For the purpose of demonstration, however, liquid-state Nuclear Magnetic Resonance (NMR) is used in this thesis as it is an ideal test-bed for developing, testing and benchmarking coherent control tools and techniques. Coherent control was revitalised in 2005 by the development of Gradient Ascent Pulse Engineering (GRAPE), a powerful optimal control technique that is widely used for designing shaped pulses for a variety of tasks. GRAPE, like any other closed-loop optimal control algorithm, requires multiple evaluations of the computationally expensive matrix exponential and the full time-evolution propagator. To this end, I present strategies to sidestep the explicit evaluation of matrix exponentials, thereby offering substantial speed-ups over conventional implementations of the GRAPE algorithm. The results are demonstrated experimentally in NMR, but also in simulations of ultracold molecules and superconducting qubits. Beyond GRAPE, this thesis also considers methods for designing spin-echo sequences for implementing any arbitrary network of controlled-Z gates in a system of qubits with zz-couplings. First, a method based on linear-programming provides near time-optimal sequences in fully-coupled systems having up to a few hundred qubits. Further, an analytic method based on graph colouring finds near time-optimal spin echo sequences in engineered systems with any number of qubits having only nearest and next-nearest neighbour-couplings.
Since no physical system can ever be completely isolated from its environment, the study of open quantum systems is pivotal to reliably and accurately control complex quantum systems. In practice, reliability of the control field needs to be confirmed via certification of the target evolution while accuracy requires the derivation of high-fidelity control schemes in the presence of decoherence. In the first part of this thesis an algebraic framework is presented that allows to determine the minimal requirements on the unique characterisation of arbitrary unitary gates in open quantum systems, independent on the particular physical implementation of the employed quantum device. To this end, a set of theorems is devised that can be used to assess whether a given set of input states on a quantum channel is sufficient to judge whether a desired unitary gate is realised. This allows to determine the minimal input for such a task, which proves to be, quite remarkably, independent of system size. These results allow to elucidate the fundamental limits regarding certification and tomography of open quantum systems. The combination of these insights with state-of-the-art Monte Carlo process certification techniques permits a significant improvement of the scaling when certifying arbitrary unitary gates. This improvement is not only restricted to quantum information devices where the basic information carrier is the qubit but it also extends to systems where the fundamental informational entities can be of arbitary dimensionality, the so-called qudits. The second part of this thesis concerns the impact of these findings from the point of view of Optimal Control Theory (OCT). OCT for quantum systems utilises concepts from engineering such as feedback and optimisation to engineer constructive and destructive interferences in order to steer a physical process in a desired direction. It turns out that the aforementioned mathematical findings allow to deduce novel optimisation functionals that significantly reduce not only the required memory for numerical control algorithms but also the total CPU time required to obtain a certain fidelity for the optimised process. The thesis concludes by discussing two problems of fundamental interest in quantum information processing from the point of view of optimal control the preparation of pure states and the implementation of unitary gates in open quantum systems. For both cases specific physical examples are considered: for the former the vibrational cooling of molecules via optical pumping and for the latter a superconducting phase qudit implementation. In particular, it is illustrated how features of the environment can be exploited to reach the desired targets.
Designing optimal control for multiparameter quantum sensing is essential for approaching the ultimate precision limits. However, analytical solutions are generally available only for simple systems, while realistic scenarios often involve coupled qubits and time-dependent Hamiltonians. Here we numerically investigate optimal control of a two-qubit sensor-ancilla system coupled via an Ising term using Gradient Ascent Pulse Engineering (GRAPE) to minimize the objective function. By seeding the optimization recursively with solutions obtained for smaller coupling strengths and selecting a suitable initial guess, we achieve robust convergence and high precision across a wide range of interaction strengths and field configurations. The proposed approach offers a practical route toward high-sensitivity, robust multiparameter magnetometry and it is applicable to solid-state quantum sensors such as nitrogen-vacancy (NV) centers in realistic experimental settings.
During the last ten years, basic quantum operations on a single electronic spins in the nitrogen-vacancy defect center in diamond have been a rich field of study. Quantum operations coherently manipulating the spin of the nitrogen-vacancy center have become promising candidates for easy to manipulate qubits. However in order to implement these qubits in quantum computers robust high-fidelity control is needed. Building on an existing confocal microscopy setup, pulsed and quadrature-amplitude modulated microwave signals were used to realize coherent spin manipulation measurements. Especially designed Smooth Optimal Control pulses (robust against detuning and different control amplitudes) were used to develop measurement schemes resulting in the aforementioned increase of fidelity. The first part of the thesis describes the implementation of these pulses into the existing experimental setup and the calibration work necessary prior to measurements, due to imperfections of devices in the microwave chain. The second part is dedicated to the analysis of the pulses applied to a single spin by comparing the experimental results to theoretical simulations. This was done not only for one resonant spin with accurate control amplitude, but also for a range of different detunings and amplitudes. A more thorough analysis of the pulses was then achieved by using state/process tomography, resulting in a complete description of the process induced by these optimized pulses. Finally, after verifying the effect of the pulses, measurement schemes for sensing alternating magnetic fields were implemented, resulting in measurements with improved sensitivity for magnetic fields.
This thesis details work performed on the improvement of experimental control of quantum systems through the use of optimal control theory. We pursue this objective through both conceptual and practical routes. We first devise improved methods of optimal control for quantum systems. We then apply them, as well as more established methods, to experimental situations where robustness to inaccuracy and error is sought. We develop a method for improving the computational efficiency of optimal control theory in the context of quantum control. This approach makes use of the iterative nature of optimisation algorithms, by using perturbation theory to minimise the effort needed to calculate the time propagator associated with a controlled Hamiltonian. We also create a new way of defining a figure of merit when optimising for robustness against error in an experiment. This method specifically applies to errors that have a relatively small effect on the controlled system's Hamiltonian. We compare this with an ensemble method based around randomly sampling several points on the control landscape, and find these methods to be largely equivalent for small errors, with the ensemble method being superior for larger error. On the applied side, we design radio frequency magnetic pulses that create robustness in spin ensembles to inhomogeneous broadening and variations of coupling strength to the control field for two applications. In the first, we create reliable gates in a situation where limitations are imposed on the control that can be applied. In the second application, we design controls for radio frequency magnetic pulses to create a superradiant state in a spin ensemble. Finally, we collaborate with the experiment to measure the electrons electric dipole moment that is being performed at Imperial College London. For this collaboration, we shape the envelope of the radio frequency control pulses used in the experiment to create superpositions of Zeeman and Stark-shifted excited states in YbF molecules. This shaping allows us to impart pre-determined phases to these superpositions, in a manner that is robust to errors in the control pulse envelope. We obtain sets of robust and sensitive pulses that have been sent to the experiment for testing purposes.
This thesis addresses challenges in the experimental realisation of optical quantum computing with atom-cavity platforms and develops techniques for experimental quantum control that generalise across a range of quantum modalities. Within the framework of cavity quantum electrodynamics (cQED), methods are developed and numerically validated for fast and precise control of single atoms to generate photonic states of interest. In particular, we consider the generation of high-repetition-rate n-photon bursts and time-bin entangled states. These photonic resources are essential for applications such as boson sampling, multi-photon interference, optical quantum computing, and quantum-enhanced metrology. Experimental improvements in coherent population transfer are demonstrated using adaptive pulse shaping with acousto-optic modulators. Beyond photon generation, the thesis introduces general-purpose pulse-level techniques, including pulse distortion correction, memory-efficient pulse compression, and machine learning-based optimisation. These methods are shown to be transferable to other platforms, such as neutral atom arrays and superconducting qubits. A particular contribution is the implementation of scalable pulse generation using fixed-point compressed pulse representations on FPGA hardware, achieving substantial memory savings while maintaining high fidelity in simulations of quantum operations. Additionally, reinforcement learning is presented as a powerful tool for optimising complex quantum dynamics, with state-of-the-art results demonstrated across various simulated systems. Throughout the thesis, theoretical developments are supported by numerical simulations and partial experimental validation, providing important insights for the development of future quantum technologies.