The pursuit of large-scale quantum computers poses two separate, though related, challenges: the need to develop robustly controllable quantum hardware; and the need to develop quantum algorithms which use it to perform meaningful compu-tations. In this thesis, we explore a selection of topics related to both of these challenges. Specifically, we focus on quantum state preparation for nuclear spin ensembles, and simu-lation algorithms for spin-orbit coupling Hamiltonians. We present a collection of indirect-measurement-based initialisation protocols for 13C baths coupled in parallel to nitrogen-vacancy defects in diamond, in a strong external field. We find that the probabilistic nature of the measurement, combined with the damaging effects of unwanted measurement outcomes, limits the utility of such protocols as means of steering the bath into some desired subspace. As a means of imparting purity into an initially incoherent bath state, the protocols appear more promising, with purity tending to increase with the number of measurements irrespective of their outcomes. We subsequently attempt to mitigate the shortcomings of these protocols by applying a corrective unitary transformation to the bath following each measurement. We find these compound protocols to indeed be capable of mapping the bath state to an arbitrary target subspace (with unit probability) given a sufficient degree of bath control; in the case where the bath control is limited, we provide lower bounds on the protocol’s success probability. We additionally show that qualitatively equivalent results can be attained using a bounded number of unitary corrections, albeit with an efficiency overhead. Finally, we turn our attention to the problem of quantum simulation, with a focus on systems possessing both spin and orbital degrees of freedom. We propose three protocols which allow the simulation of arbitrary spin-orbit coupling interactions using a model system undergoing a controlled discrete-time quantum walk (DTQW). The number of DTQW steps required to execute this simulation is found to be at most quadratic in the dimension of the simulated Hilbert space.
The pursuit of large-scale quantum computers poses two separate, though related, challenges: the need to develop robustly controllable quantum hardware; and the need to develop quantum algorithms which use it to perform meaningful compu-tations. In this thesis, we explore a selection of topics related to both of these challenges. Specifically, we focus on quantum state preparation for nuclear spin ensembles, and simu-lation algorithms for spin-orbit coupling Hamiltonians. We present a collection of indirect-measurement-based initialisation protocols for 13C baths coupled in parallel to nitrogen-vacancy defects in diamond, in a strong external field. We find that the probabilistic nature of the measurement, combined with the damaging effects of unwanted measurement outcomes, limits the utility of such protocols as means of steering the bath into some desired subspace. As a means of imparting purity into an initially incoherent bath state, the protocols appear more promising, with purity tending to increase with the number of measurements irrespective of their outcomes. We subsequently attempt to mitigate the shortcomings of these protocols by applying a corrective unitary transformation to the bath following each measurement. We find these compound protocols to indeed be capable of mapping the bath state to an arbitrary target subspace (with unit probability) given a sufficient degree of bath control; in the case where the bath control is limited, we provide lower bounds on the protocol’s success probability. We additionally show that qualitatively equivalent results can be attained using a bounded number of unitary corrections, albeit with an efficiency overhead. Finally, we turn our attention to the problem of quantum simulation, with a focus on systems possessing both spin and orbital degrees of freedom. We propose three protocols which allow the simulation of arbitrary spin-orbit coupling interactions using a model system undergoing a controlled discrete-time quantum walk (DTQW). The number of DTQW steps required to execute this simulation is found to be at most quadratic in the dimension of the simulated Hilbert space.
This thesis presents a collection of projects spanning different sub-fields of quantum science, undertaken with the goal of understanding and advancing quantum technologies. Broadly, it can be divided into two thematic parts — parameter estimation and open system dynamics. Each project addresses inverse and ill-posed problems in Physics, which lie at the heart of developing robust and scalable quantum devices.A central theme in quantum technology is the challenge of inference of microscopic system parameters from limited, indirect observations. The first part of the thesis investigates this through the problem of Hamiltonian reconstruction via local measurements. Indirect estimation of couplings in quantum systems relies on the measurement of the spectrum and the overlap of eigenvectors with some reference state. For a one-dimensional chain, this data can be obtained by local measurement on one end of the chain, thereby reducing the need for full Hamiltonian tomography. Information about couplings is extracted from the temporal data obtained by measuring the expectation values of the time evolution 𝑒−𝑖𝐻𝑡 for a reference state. In Chapter 3, we analyze the robustness of this estimation scheme under perturbations arising from beyond nearest neighbour interactions. We show that the error scales linearly with the strength of such interactions and on average, the error increases with the distance of interaction between sites.Chapter 4 examines whether coupling information can be extracted from local thermal measurements, using expectation values of the Gibbs state at varying temperatures rather than temporal data. We develop a procedure to obtain the coefficients of the Taylor expansion of these expectation values and relate them to the Hamiltonian parameters. For very small chains, this mapping can be carried out analytically, while for larger systems it reveals the algebraic structure that links local measurements to the underlying couplings and highlights the trade-offs between measurement resources, numerical stability, and identifiability. The analysis also clarifies how additional local fields or self-interaction terms enhance the information content of thermal data, suggesting a role for local thermal probes as practical tools for Hamiltonian verification and parameter estimation.Building on the ideas of controlling and inferring information about a quantum system, we now turn to active intervention through adaptive measurement. In Chapter 5, we develop a process tensor driven procedure for cooling the spin bath that is coupled to a nitrogen vacancy (NV) center in diamond. By modeling the sequence of intermediate quantum instruments acting on a correlated system-environment process, we optimize a pair of completely positive (CP) maps to maximize the population in a lower-energy state. Unlike existing approaches that rely solely on positive operator valued measures (POVMs), our method encompasses a broader class of CP maps, including adaptive feed-forward and mixed operations. We explicitly account for initial correlation between system and environment and distinguish between the controllable and uncontrollable parts of the dynamics. Our framework supports non-Markovian operations and benchmarks them against optimal Markovian strategies. The optimization is performed via Semi-definite Programming (SDP), ensuring global optimality. We also assess robustness to Hamiltonian noise and provide a proposal for implementation using NV center in diamonds.Finally, Chapter 6 explore the relaxation dynamics of topological qubits, focusing on a tetron qubit formed from two uncoupled Kitaev chains coupled to a finite fermionic bath. Using the correlation matrix formalism for purely quadratic couplings, we show that the relaxation is fundamentally independent of temperature when either the bath is large, or the zero-mode energy of the system is close to zero. This challenges a key assumption in the field that cooling enhances coherence. Interestingly, we find that introducing glassy disorder into the system slows down relaxation, offering a potential route to prolong qubit lifetimes.Collectively, these studies form a coherent narrative around extraction, control and utilization of quantum information under fundamental constraints. By tackling such inverse and often ill-posed problems, this thesis contributes new tools and insights essential for the realization of future quantum technologies.
Digital information based on the laws of quantum mechanics promisses powerful new ways of computation and communication. However, quantum information is very fragile; inevitable errors continuously build up and eventually all information is lost. Therefore, realistic large-scale quantum information processing requires the protection of quantum bits (qubits) against errors. In this thesis we present the experimental implementation of quantum error correction protocols based on spins in diamond. In such protocols, a quantum state is protected against errors by encoding in multiple qubits. Errors can be detected and corrected by measurement of correlations, so-called stabilizer-measurements, on these qubits.The experimental work presented in this thesis employs multiple spins in diamond as qubits to explore and implement error correction protocols. The nitrogen-vacancy (NV) centre in diamond is a lattice defect consisting of a nitrogen atom (N) and a vacancy (V) on two adjacent diamond lattice sites. This defect effectively results in an electronic spin that can be addressed as a qubit. The spin state can be manipulated by microwave fields and optically read out. At liquid helium temperatures (cryogenic temperature, ~4 K = -269 C), the NV electron spin provides high-fidelity single-shot readout and long coherence times.The NV centre is surrounded by naturally available (1.1% abundance) nuclear C13 spins. As the number of spins that are close enough to the NV centre to be strongly coupled is limited, we employ the weakly coupled nuclear spins in the spin bath of the NV centre. Using dynamical decoupling techniques these nuclear spins can be detected via the NV electron spin through the hyperfine interaction. The nuclear spins are long-lived and robust against optical excitation of the NV electron spin, which can make these spins a robust quantum register for quantum error correction.In Ch. 4 we demonstrate universal control over multiple of such weakly coupled nuclear C13 spins in the environment of the NV centre at ambient temperatures. We demonstrate initialization, control and read-out of individual nuclear spins. Finally, we implement a quantum error correction protocol by encoding a quantum state in the NV electron spin and two nuclear spins. Errors are detected by un-encoding the quantum state back to the electron spin and correction via a double controlled operation.For universal fault-tolerant quantum computations it is essential that the quantum information remains encoded at all times. In Ch. 5 we present multiple rounds of quantum error correction and active feedback on a continuously encoded qubit at cryogenic temperatures. A quantum state is protected by encoding in three weakly coupled spins. Errors are detected via high-fidelity non-demolition readout of the NV electron spin and actively corrected using fast classical electronics. We demonstrate that an actively error-corrected qubit is robust against phase flip errors and show that a superposition state can live longer than the best physical qubit in the encoding.The presented methods and results can be extended to a range of future experiments. In Ch. 6 we propose the implementation of five-qubit quantum error correction, the smallest code to correct for general single-qubit errors on the physical qubits in the encoding, by extending the experimental methods as developed in Chs. 4&5. Besides the exploration and development of larger error correction protocols and fault-tolerant quantum computing, the presented quantum register based in spins in diamond can be employed as a quantum node and combined with recent advances in the realization of quantum entanglement over large distances to form quantum networks. These networks can be used to study both fundamental questions as well as future applications in quantum information technology.
The study of quantum many-body systems is crucial to our understanding of nature at the microscopic scale. As analytical solutions quickly become intractable, the development of efficient computational simulation techniques is indispensable to predict the behaviour of quantum systems. This task is particularly challenging as the dimension of the underlying Hilbert space grows exponentially with the system size. While classical computational methods have achieved remarkable success in specific regimes, their applicability is fundamentally limited by this exponential scaling. Quantum computers offer a natural platform for representing and simulating quantum systems, but current devices are constrained by noise and limited qubit counts, drastically restricting the algorithms that can be run. In this context, hybrid quantum-classical algorithms provide a promising approach to combine the strengths of both paradigms. This thesis develops hybrid quantum-classical algorithms for the simulation of quantum many-body systems. The key idea is to perform classically difficult tasks on near-term quantum devices, while leveraging classical computational power to control, correct, and extend the obtained results. Within this framework, we introduce two complementary approaches for the simulation of quantum dynamics. The first method employs circuit knitting techniques to distribute variational quantum simulations across multiple quantum devices. The entanglement between weakly coupled clusters of highly correlated spins is recovered in classical post-processing, where the overhead is controlled through a constrained optimisation problem. The second method combines a simplified, Trotterised quantum dynamics simulation with a parametrised classical ansatz trained to correct for the approximations made on the quantum device. We show that this method can be employed to correct Trotter errors, implement long-range gates with hardware-efficient circuits, or simulate larger systems by incorporating additional degrees of freedom purely classically. In addition, we present a hybrid approach to computing thermal properties of quantum many-body systems via the Quantum Finite Temperature Lanczos Method. A Krylov subspace is generated on a quantum computer by combining the efficient preparation of typical states with real-time evolution. A classical computer then diagonalises the system in the low-dimensional subspace and estimates the finite-temperature expectation values through trace estimation. The results presented in this thesis demonstrate that hybrid quantum-classical algorithms can expand the range of systems that can be studied on near-term quantum devices. Conversely, we show that incorporating quantum subroutines into classical simulation techniques can improve their efficiency. These results suggest that, rather than treating classical and quantum simulation as competing paradigms, their careful integration can provide a more effective route toward practical quantum many-body simulation.
A functioning qubit must be able to be initialized and measured. The fidelity of these operations is essential for all quantum applications, including quantum sensing, communication, and computation. The diamond nitrogen-vacancy (NV) center is a point defect in the lattice with an optical interface to a coherent ground-state spin, which makes the NV center one of the few spin qubits operable at room temperature. While the NV center spin state can be initialized and read out optically, the fidelity of these operations are far from perfect due to the charge and orbital dynamics. In typical conditions, the NV center is in the proper charge state 75% of the time, and measuring the spin state results in a non-zero signal only 1% of the time. These inefficient mechanisms make many measurements practically intractable. This thesis focuses on improving the preparation and measurement fidelities of NV centers through precise all-optical control of the charge, orbital, and spin dynamics. I first discuss an improved spin readout mechanism which relies on spin-to-charge conversion (SCC) and discuss the potential for single-shot spin readout. Following, I present how charge readout and SCC can be implemented in ensembles of NV centers within nanodiamonds and demonstrate that it provides improvements for spin-relaxometry studies. Finally, I develop a method for initializing a single NV center's charge state with real-time control and show that this capability improves spin readout performance for sensing. To conclude, I discuss how these improved initialization and readout capabilities can be applied to detecting and controlling coupled nuclear spins in the diamond lattice and consider other applications of real-time control.
Since its introduction one decade ago, the quantum algorithm for chemistry has been among the most anticipated applications of quantum computers. However, as the age of industrial quantum technology dawns, so has the realization that even “polynomial” resource overheads are often prohibitive. There remains a large gap between the capabilities of existing hardware and the resources required to quantum compute classically intractable problems in chemistry. The primary contribution of this dissertation is to take meaningful steps towards reducing the costs of three approaches to quantum computing chemistry. First, we discuss how chemistry problems can be embedded in Hamiltonians suitable for commercially manufactured quantum annealing machines. We introduce schemes for more efficiently compiling problems to annealing Hamiltonians and apply the techniques to problems in protein folding, gene expression, and cheminformatics. Second, we introduce the first adiabatic quantum algorithm for fermionic simulation. Towards this end, we develop tools which embed arbitrary universal Hamiltonians in constrained hardware at a reduced cost. Finally, we turn our attention to the digital quantum algorithm for chemistry. By exploiting the locality of physical interactions, we quadratically reduce the number of terms which must be simulated. By analyzing the scaling of time discretization errors in terms of chemical properties, we obtain significantly tighter bounds on the minimum number of time steps which must be simulated. Also included in this dissertation is a protocol for preparing configuration interaction states that is asymptotically superior to all prior results and the details of the most accurate experimental quantum simulation of chemistry ever performed.
Thermal state preparation is a central challenge in the simulation of quantum many-body systems. Yet, provably efficient algorithms for this task were only introduced recently [Chen et al. Nature 646, 561 (2025)]. These algorithms are based on dissipative Lindbladian evolution which exactly fixes the thermal state. Controlled and efficient digital simulation of this evolution, although possible in principle, remains out of reach for present-day quantum hardware. Subsequent work has therefore focused on analog approximations of the proposed Lindbladians via `collision models' with relatively modest requirements -- a resettable bath of ancilla qubits whose couplings to the system can be tuned in time-dependent fashion -- while still admitting rigorous fixed-point error bounds. Existing rigorous approaches, however, do not exploit the fact that these constructions generically implement not only the desired Lindblad dynamics, but also an additional unitary evolution generated by the system Hamiltonian which may aid convergence to the thermal state [Lloyd and Abanin arXiv:2506.21318 (2025)]. Here, we show that this unitary contribution does indeed tighten the fixed-point error bound and demonstrate that it is rigorously controlled by the system-bath coupling strength J, scaling as J2. This demonstrates that the effect of the spurious `Lamb shift' term generated by the system-bath interaction can be controlled by tuning J. We clarify the role, previously observed, of a randomized implementation in suppressing possible resonances of the drive with the many-body spectrum, and bound the additional variance that this randomization imposes on observables. Finally, we numerically study aspects of the protocol which are relevant for its practical realization, such as the mixing time.