Nitrogen-vacancy (NV) center ensembles have the potential to improve a wide range of applications, including nuclear magnetic resonance spectroscopy at the microscale and nanoscale, wide-field magnetometry, and hyperpolarization of nuclear spins via the transfer of optically induced NV polarization to nearby nuclear spin clusters. These NV ensembles can be coherently manipulated with microwave cavities, that deliver strong and homogeneous drivings over large volumes. However, the pulse shaping for microwave cavities presents the challenge that the external controls and intracavity field amplitudes are not identical, leading to adverse effects on the accuracy of operations on the NV ensemble. In this paper, we introduce a method based on gradient ascent pulse engineering (GRAPE) to optimize external controls, resulting in robust pulses within the cavity while minimizing the effects of cavity ringings. The effectiveness of the method is demonstrated by designing both π and π / 2 pulses. These optimized controls are then integrated into a PulsePol sequence, where numerical simulations reveal a resilience to detunings five times larger than those tolerated by the sequence constructed using standard controls.
Nitrogen-vacancy (NV) center ensembles have the potential to improve a wide range of applications, including nuclear magnetic resonance spectroscopy at the microscale and nanoscale, wide-field magnetometry, and hyperpolarization of nuclear spins via the transfer of optically induced NV polarization to nearby nuclear spin clusters. These NV ensembles can be coherently manipulated with microwave cavities, that deliver strong and homogeneous drivings over large volumes. However, the pulse shaping for microwave cavities presents the challenge that the external controls and intracavity field amplitudes are not identical, leading to adverse effects on the accuracy of operations on the NV ensemble. In this paper, we introduce a method based on gradient ascent pulse engineering (GRAPE) to optimize external controls, resulting in robust pulses within the cavity while minimizing the effects of cavity ringings. The effectiveness of the method is demonstrated by designing both π and π / 2 pulses. These optimized controls are then integrated into a PulsePol sequence, where numerical simulations reveal a resilience to detunings five times larger than those tolerated by the sequence constructed using standard controls.
Nitrogen-vacancy (NV) centers in diamond are a leading platform for vector magnetometry, offering intrinsic sensitivity to both the magnitude and direction of magnetic fields. NV magnetometers typically rely on an external bias field to lift the degeneracy of the ground-state spin sublevels, enabling spectral discrimination of different NV orientations and spin transitions. At high accuracy, however, such a bias field systematically introduces errors through thermal, mechanical, and hysteretic drifts, thus hindering the accurate measurement of the magnetic field of interest. Several strategies have been proposed to address this limitation, including optical polarization-based orientation labeling, optical anisotropy, strong coupling to nearby nuclear spins, circular microwave polarization, and tailored pulse sequences. In this work, we introduce an optimization-based pulse-shaping control framework that enables selective and robust manipulation of NV ensembles without relying on a static bias field. Our method achieves both orientation-selective and subspace-selective control through optimal temporal modulation of the driving fields, providing a route to resolving spectral overlaps in degenerate NV systems.
Numerical optimizations of the microwave and radio frequency control pulses for the nitrogen vacancy electron-nuclear spin register were performed by means of a gradient ascent pulse engineering method (GRAPE). Three examples of spin control — specific quantum state preparation and the implementation of a controlled-NOT and unconditional - gate have been optimized through parallel computation. The optimized control pulses reach fidelities of F = 0:99944, F = 0:77929 and F = 0:99143 respectively, whereas simulation of Rabi oscillation based control yields corresponding results of F = 0:96325, F = 0:21884 and F = 0:42702. The fixed step size in the GRAPE algorithm imposes a tradeoff between monotone and fast convergence of optimized control pulses and the unspecific performance function may lead to erroneous optimizations. These complications require future research to be resolved. Furthermore, implementing the effect of decoherence yields no significant average fidelity improvement, but has a positive effect on reducing the spread of final density states for the case of quantum state preparation.
Defects in solid-state materials provide an ideal, robust platform for quantum sensing. To deliver maximum sensitivity, a large ensemble of noninteracting defects hosting quantum states with long coherence is required. Control of such an ensemble is challenging due to the spatial variation in both the defect energy levels and in any control field across a macroscopic sample. In this work, we experimentally demonstrate that we can overcome these challenges using Floquet theory and optimal control optimization methods to efficiently and coherently control a large defect ensemble, suitable for sensing. We apply our methods experimentally to a spin ensemble of up to $4\ifmmode\times\else\texttimes\fi{}{10}^{9}$ nitrogen-vacancy centers in diamond. By explicitly including the hyperfine interaction to the intrinsic 14N nuclear spin in the optimization, we design shaped microwave control pulses that can outperform conventional ($\ensuremath{\pi}$) pulses when applied to sensing schemes, with an improvement in the strength of ensemble response of between 11% and 78%. Through simulation of the ensemble dynamics, we shed light on the bandwidth limitations of large-ensemble reinitialization and propose alternative routes for further improvement.
The homogeneity of the microwave magnetic field is essential in controlling a large volume of ensemble spins, for example, in the case of sensitive magnetometry with nitrogen-vacancy (NV) centers in diamond. This is particularly important for pulsed measurement, where the fidelity of control pulses plays a crucial role in its sensitivity. So far, several magnetic field-forming systems have been proposed, but no detailed comparison has been made. Here, we numerically study the homogeneity of five different systems, including a planar antenna, a dielectric resonator, a cylindrical inductor, a barrel-shaped coil, and a nested barrel-shaped coil. The results of the simulation allowed us to optimize the design parameters of the barrel-shaped field-forming system, which led to significantly improved magnetic field uniformity. To measure this effect, we experimentally compared the homogeneity of a field-forming system having a barrel shape with that of a planar field-forming system by measuring Rabi oscillations of an ensemble of NV centers with them. Significant improvements in inhomogeneity were confirmed in the barrel-shaped coil.
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.
PulsePol is an elegantly designed pulse-sequence-based quantum control scheme that enables polarization transfer between electron and nuclear spins, for example, in nitrogen-vacancy (NV) centers. However, previous analyses of PulsePol assumed very strong, near-ideal, instantaneous microwave pulses, which is rarely achievable at higher magnetic fields. We revisit the PulsePol scheme under finite-pulse constraints and show that its performance significantly degrades due to finite-pulse effects. Using bimodal Floquet theory, we identify the symmetry-breaking mechanism responsible for this deterioration in fidelity. By phase adjustment, we reestablish the proper symmetry of the interaction-frame spin Hamiltonian, leading to a sequence called Q-PulsePol, where "Q" reflects the restored quadrature symmetry. Our results demonstrate robustness to finite-pulse effects and improved polarization transfer efficiency, establishing Q-PulsePol as a practical and reliable scheme for bulk hyperpolarization of nuclear spins in solids using a single-mode (zero-quantum or double-quantum) transfer. This work bridges idealized quantum control with realistic pulse engineering, establishing design rules for spin-based quantum control protocols.