State of the art quantum sensing experiments targeting frequency measurements or frequency addressing of nuclear spins require one to drive the probe system at the targeted frequency. In addition, there is a substantial advantage to performing these experiments in the regime of high magnetic fields, in which the Larmor frequency of the measured spins is large. In this scenario we are confronted with a natural challenge of controlling a target system with a very high frequency when the probe system cannot be set to resonance with the target frequency. In this contribution we present a set of protocols that are capable of confronting this challenge, even at large frequency mismatches between the probe system and the target system, both for polarization and for quantum sensing.
State of the art quantum sensing experiments targeting frequency measurements or frequency addressing of nuclear spins require one to drive the probe system at the targeted frequency. In addition, there is a substantial advantage to performing these experiments in the regime of high magnetic fields, in which the Larmor frequency of the measured spins is large. In this scenario we are confronted with a natural challenge of controlling a target system with a very high frequency when the probe system cannot be set to resonance with the target frequency. In this contribution we present a set of protocols that are capable of confronting this challenge, even at large frequency mismatches between the probe system and the target system, both for polarization and for quantum sensing.
In recent years, the field of quantum sensing has garnered increasing attention due to its potential to revolutionize various scientific and technological domains. Among the different quantum sensors, the nitrogen-vacancy (NV) color center in diamond stands out for its ease of use, ability to be read out and initialized with a laser, and long coherence times even at room temperature. Over the past years, numerous quantum control sequences have been developed to successfully deploy NV sensors in diverse situations, such as measuring nearby spin clusters, classical AC signals, and static magnetic fields. However, the NV center faces limitations when coupling to high frequency signals. More specifically, as the frequency of the target signal increases, stronger driving fields over NVs are needed, ultimately reaching the limits of current experimental capabilities. In this thesis, we propose several protocols to address this high-frequency problem in different scenarios.
We study control of electron-nuclear spin dynamics at magnetic field strengths where the Larmor frequency of the nucleus is comparable to the hyperfine coupling strength. The quantization axis for the nuclear spin differs from the static B0 field direction and depends on the state of the electron spin. The quantization axis can be switched by flipping the state of electron spin, allowing for universal control of nuclear spin states. We show that by performing a sequence of flips (each followed by a suitable delay), we can perform any desired rotation of the nuclear spin, which can also be conditioned on the state of the electron spin. These operations, combined with electron spin rotations, can be used to synthesize any unitary transformation of the coupled electron-nuclear spin system. We discuss how these methods can be used for design of experiments for transfer of polarization from the electron to the nuclear spins.
Quantum sensing utilizes the quantum resources of well-controlled quantum systems to measure small signals with high sensitivity, and has great potential in both fundamental science and concrete applications. Interacting quantum systems have attracted increasing interest in the field of precise measurements, owing to their potential to generate quantum-correlated states and exhibit rich many-body dynamics. These features provide a novel avenue for exploiting quantum resources in sensing applications. Although previous studies have shown that using such systems can improve sensitivity, they mainly focused on measuring individual physical quantities. In experiment, the challenge of using interacting quantum systems to achieve high-precision measurements of multiple physical parameters simultaneously has not been explored to a large extent. In this study, we demonstrate a first realisation of interaction-based multiparameter sensing by using strongly interacting nuclear spins under ultra-low magnetic field conditions. We find that, as the interaction strength among nuclear spins becomes significantly larger than their Larmor frequencies, a different regime emerges where the strongly interacting spins can be simultaneously sensitive to all components of a multidimensional field, such as a three-dimensional magnetic field. Moreover, we observe that the strong interactions between nuclear spins can increase their quantum coherence times to as long as several seconds, thereby improving measurement precision. Our sensor successfully achieves precision measurement of three-dimensional vector magnetic fields with a field sensitivity reaching the order of 10–11 T and an angular resolution as high as 0.2 rad. Importantly, this approach eliminates the need for external reference fields, thereby avoiding calibration errors and technical noise commonly encountered in traditional magnetometry. Experimentally optimized protocol further enhances the sensitivity of the interacting spin-based sensor by up to five orders of magnitude compared with non-interacting or classical schemes. These results demonstrate the enormous potential of interacting spin systems as a powerful platform for high-precision multi-parameter quantum sensing. The techniques developed here pave the way for a new generation of quantum sensors that use intrinsic spin interactions to exceed the traditional sensitivity limits, presenting a promising route toward ultra-sensitive, calibration-free magnetometry in complex environments.
The ability to perform quantum error correction (QEC) arbitrarily many cycles is a significant challenge for scalable quantum information processing (QIP). Key requirements for multiple-round QEC are a high degree of quantum control, the ability to efficiently characterize both intrinsic and extrinsic noise, and the ability to dynamically and efficiently extract entropy from ancilla qubits. Nuclear Magnetic Resonance (NMR) based quantum devices have demonstrated high control fidelity with up to 12 qubits, and the noise characterizations can be performed using an efficient protocol known as randomized benchmarking. One of the remaining challenges with NMR systems is that qubit initialization is normally only attainable via thermal equilibration. This results in very low polarizations in reasonable experimental conditions. Moving to electron-nuclear coupled spin systems in a single crystal is a promising solution to the ancilla qubit preparation problem. One obvious advantage of incorporating electron spins comes from higher gyromagnetic ratio of the electron which yields about three orders of magnitude larger thermal spin polarization than that of nuclear spins in the same experimental condition. In addition, fast control of nuclear spins is possible provided appropriate level of anisotropic hyperfine interaction strength. The nuclear spins can be polarized even beyond the thermal electron spin temperature using a technique Heat-Bath Algorithmic Cooling (HBAC). With theoretical ideas in hand, the next step is to develop classical instrumentations to control electron-nuclear coupled systems and accomplish high fidelity coherent control. Noise characterizations are also necessary for benchmarking the quality of control over the electron-nuclear spin system. \nI first present example applications of NMR QIP with small number of qubits: Testing a foundational question in quantum mechanics and measuring spectral density of noise in a quantum system. Then I report on our home-built X-band electron spin resonance (ESR) spectrometer and progress in achieving high fidelity coherent control of electron and nuclear spins for QIP. We focus on implementing nuclear spin manipulation via anisotropic hyperfine interaction and microwave (mw) control, but discussions also include electron nuclear double resonance (ENDOR) control techniques. We perform realistic algorithmic simulations to show that an experimental cooling of nuclear spins below electron thermal temperature is feasible, and to present the electron-nuclear spin systems as promising testbeds for scalable QIP.
The use of nuclear spins as physical sensing systems is disadvantaged by their low signal responsivity, particularly when compared to sensing techniques based on electron spins. This primarily results from the small nuclear gyromagnetic ratio and the difficulties in achieving high spin polarization. Here we develop a new approach to investigating the response of hyperpolarized molecular nuclear spins to magnetic fields and demonstrate orders-of-magnitude enhanced magnetic responsivity over state-of-the-art proton and Overhauser magnetometers. Using hyperpolarized molecules with proton spins, we report the realization of magnetic amplification in linear and nonlinear types. We further extend this amplification to hyperpolarized scalar-coupled multi-spin molecules and observe substantial magnetic amplification exceeding 10%. Moreover, we observe an anomalous amplification with dispersive frequency dependence that originates from magnetic interference effects. Our work highlights the potential of hyperpolarized molecular nuclear spins for use in a new class of quantum sensors, with promising applications in both applied and fundamental physics, including highly accurate absolute magnetometry and the exploration of axion-nucleon exotic interactions.
The goal of this project was to improve our control over nuclear spins in the solid state, and to extend this control to coupled electron-nuclear spins. Our key results are summarized below. 1. We extended the control techniques developed in liquid state NMR quantum information processing to the control of a three-qubit solid state NMR quantum information processor. 2. To explore multi-body spin dynamics and their sensitivity to decoherence, we have measured the decay of NMR multiple quantum coherence intensities in the presence and absence of the dipolar Hamiltonian, in a cubic and a one-dimensional spin system. 3. We also studied the transport of polarization in the one-dimensional fluoroapatite system, both experimentally and theoretically, and created special states in which the polarization is localized to the ends of the chain. This enables both universal Quantum Computing and Quantum Simulation in 1-D systems. 4. We devised a novel scheme for electron-nuclear quantum information processing that exploits the anisotropic hyperfine coupling. This scheme enables universal control over a 1-electron, N-nuclear spin system, addressing only a single electron spin transition. Not having to address the nuclear spins directly significantly speeds up the control. We designed and fabricated a pulsed electron spin resonance spectrometer, along with a cryogenic probe which we used to experimentally implement this scheme on a single crystal sample of irradiated malonic acid. 5. We demonstrated the role of nuclear spin dipolar diffusion in dynamic nuclear polarization (DNP) experiments, in dielectric samples with abundant nuclear spins. We achieved a 29Si polarization of 8.3% at 66 GHz and 1.1 K in single crystal P-doped, the highest ever reported, using DNP.