arXiv subjects

Liam T. Hall

Publications and source records attributed to Liam T. Hall.

18 recordsLinked to original sources

arXiv2026

A method for robust spin relaxometry in the presence of imperfect state preparation

Spin relaxometry based on quantum spin systems has developed as a valuable tool in medical and condensed matter systems, offering the advantage of operating without the need for external DC or RF fields. Spin relaxometry with nitrogen-vacancy (NV) centers has been applied to paramagnetic sensing using both single crystal diamond and nanodiamond materials. However, these methods often suffer from artifacts and systematic uncertainties, particularly due to imperfect spin state preparation, leading to artificially fast T$_1$ relaxation times. Current analysis techniques fail to adequately account for these issues, limiting the precision of parameter estimation. In this work, we introduce a minimal fitting procedure that enables more robust parameter estimation in the presence of imperfect spin polarization. Our model improves upon existing approaches by offering more accurate fits and provides a framework for efficiently parallelizing single-spin dynamics studies.

quant-ph↗

arXiv2023

Quantum diamond magnetometry for navigation in GNSS denied environments

In this paper, a probabilistic method for map matching localisation based on magnetometery measurement and total magnetic intensity maps is described. We show that the method is able to effectively address the challenge issues associated with map matching using geophysical maps and provides a mechanism of handling map measurement ambiguity and a way of evaluating the underlying quality. Furthermore, the effectiveness of the magnetometery map matching localisation is demonstrated using the simulation of removing position drift of an inertial navigation system, that arises in INS over a long duration, by the magnetometery aiding in the absence GNSS positioning. Simulation results using online maps verified the robustness and effectiveness of the proposed algorithm, particularly, the aiding precision will be getting better if a high sensitivity magnetometer is used.

math.OC↗

arXiv2022

Method for in-solution, high-throughput T1 relaxometry using fluorescent nanodiamonds

Fluorescent nanodiamonds (FNDs) have been exploited as sensitive quantum probes for nanoscale chemical and biological sensing applications, with the majority of demonstrations to date relying on the detection of single FNDs. This places significant limits on the measurement time, throughput and statistical significance of a measured result as there is usually marked inhomogeneity within FND samples. Here we have developed a measurement platform that can report the T1 spin relaxation time from a large ensemble of FNDs in solution. We first describe a refined sensing protocol for this modality and then use it to identify the optimal FND size for the detection of paramagnetic targets. Our approach is simple to set up, robust and can be used for rapid material characterisation or a variety of in-situ quantum sensing applications.

quant-ph↗

arXiv2019

Quantum magnetic imaging of iron biomineralisation in teeth of the chiton Acanthopleura hirtosa

Iron biomineralisation is critical for life. Nature capitalises on the physical attributes of iron biominerals for a variety of functional, structural and sensory applications. Although magnetism is an integral property of iron biominerals, the role it plays in their nano-assembly remains a fundamental, unanswered question. This is well exemplified by the magnetite-bearing radula of chitons. Chitons, a class of marine mollusc, create the hardest biomineral of any animal in their abrasion-resistant, self-sharpening teeth4. Despite this system being subjected to a range of high resolution imaging studies, the mechanisms that drive mineral assembly remain unresolved. However, the advent of quantum imaging technology provides a new avenue to probe magnetic structures directly. Here we use quantum magnetic microscopy, based on nitrogen-vacancy centres in diamond, to attain the first subcellular magnetic profiling of a eukaryotic system. Using complementary magnetic imaging protocols, we spatially map the principal mineral phases (ferrihydrite and magnetite) in the developing teeth of Acanthopleura hirtosa with submicron resolution. The images reveal previously undiscovered long-range magnetic order, established at the onset of magnetite mineralisation. This is in contrast to electron microscopy studies that show no strong common crystallographic orientation. The quantum-based magnetic profiling techniques presented in this work have broad application in biology, earth science, chemistry and materials engineering and can be applied across the range of systems for which iron is vital.

physics.bio-ph↗

arXiv2018

Non-neurotoxic Nanodiamond Probes for Intraneuronal Temperature Mapping

Optical bio-markers have been used extensively for intracellular imaging with high spatial and temporal resolution. Extending the modality of these probes is a key driver in cell biology. In recent years, the NV centre in nanodiamond has emerged as a promising candidate for bio-imaging and bio-sensing with low cytotoxicity and stable photoluminescence. Here we study the electrophysiological effects of this quantum probe in primary cortical neurons. Multi-electrode array (MEA) recordings across five replicate studies showed no statistically significant difference in 25 network parameters when nanodiamonds are added at varying concentrations over various time periods 12-36 hr. The physiological validation motivates the second part of the study which demonstrates how the quantum properties of these biomarkers can be used to report intracellular information beyond their location and movement. Using the optically detected magnetic resonance from the nitrogen vacancy defects within the nanodiamonds we demonstrate enhanced signal-to-noise imaging and temperature mapping from thousands of nanodiamond probes simultaneously. This work establishes nanodiamonds as viable multi-functional intraneuronal sensors with nanoscale resolution, that may ultimately be used to detect magnetic and electrical activity at the membrane level in excitable cellular systems.

physics.bio-ph↗

arXiv2017

High precision single qubit tuning via thermo-magnetic field control

Precise control of the resonant frequency of a spin qubit is of fundamental importance to quantum sensing protocols. We demonstrate a control technique on a single nitrogen-vacancy (NV) centre in diamond where the applied magnetic field is modified by fine-tuning a permanent magnet's magnetisation via temperature control. Through this control mechanism, nanoscale cross-relaxation spectroscopy of both electron and nuclear spins in the vicinity of the NV centre are performed. We then show that through maintaining the magnet at a constant temperature an order of magnitude improvement in the stability of the NV qubit frequency can be achieved. This improved stability is tested in the polarisation of a small ensemble of nearby $^{13}$C spins via resonant cross-relaxation and the lifetime of this polarisation explored. The effectiveness and relative simplicity of this technique may find use in the realisation of portable spectroscopy and/or hyperpolarisation systems.

quant-ph↗

arXiv2017

Quantum probe hyperpolarisation of molecular nuclear spins

The hyperpolarisation of nuclear spins within target molecules is a critical and complex challenge in magnetic resonance imaging (MRI) and nuclear magnetic resonance (NMR) spectroscopy. Hyperpolarisation offers enormous gains in signal and spatial resolution which may ultimately lead to the development of molecular MRI and NMR. At present, techniques used to polarise nuclear spins generally require low temperatures and/or high magnetic fields, radio-frequency control fields, or the introduction of catalysts or free-radical mediators. The emergence of room temperature solid-state spin qubits has opened exciting new pathways to circumvent these requirements to achieve direct nuclear spin hyperpolarisation using quantum control. Employing a novel cross-relaxation induced polarisation (CRIP) protocol using a single nitrogen-vacancy (NV) centre in diamond, we demonstrate the first external nuclear spin hyperpolarisation achieved by a quantum probe, in this case of $^1$H molecular spins in poly(methyl methacrylate). In doing so, we show that a single qubit is capable of increasing the thermal polarisation of $\sim 10^6$ nuclear spins by six orders of magnitude, equivalent to an applied magnetic field of $10^5$\,T. The technique can also be tuned to multiple spin species, which we demonstrate using both \C{13} and $^1$H nuclear spin ensembles. Our results are analysed and interpreted via a detailed theoretical treatment, which is also used to describe how the system can be scaled up to a universal quantum hyperpolarisation platform for the production of macroscopic quantities of contrast agents at high polarisation levels for clinical applications. These results represent a new paradigm for nuclear spin hyperpolarisation for molecular imaging and spectroscopy, and beyond into areas such as materials science and quantum information processing.

quant-ph↗

arXiv2017

Quantum magnetic resonance microscopy

Magnetic resonance spectroscopy is universally regarded as one of the most important tools in chemical and bio-medical research. However, sensitivity limitations typically restrict imaging resolution to length scales greater than 10 μm. Here we bring quantum control to the detection of chemical systems to demonstrate high resolution electron spin imaging using the quantum properties of an array of nitrogen-vacancy (NV) centres in diamond. Our quantum magnetic resonance microscope selectively images electronic spin species by precisely tuning a magnetic field to bring the quantum probes into resonance with the external target spins. This provides diffraction limited spatial resolution of the target spin species over a field of view of ~50x50 μm^2. We demonstrate imaging and spectroscopy on aqueous Cu2+ ions over microscopic volumes (0.025 μm^3), with detection sensitivity at resonance of 104 spins/voxel, ~100 zeptomol (10^-19 mol). The ability to image, perform spectroscopy and dynamically monitor spin-dependent redox reactions and transition metal biochemistry at these scales opens up a new realm of nanoscopic electron spin resonance and zepto-chemistry in the physical and life sciences.

physics.bio-ph↗

arXiv2016

Microwave-Free Nuclear Magnetic Resonance at Molecular Scales

The implementation of nuclear magnetic resonance (NMR) at the nanoscale is a major challenge, as conventional systems require relatively large ensembles of spins and limit resolution to mesoscopic scales. New approaches based on quantum spin probes, such as the nitrogen-vacancy (NV) centre in diamond, have recently achieved nano-NMR under ambient conditions. However, the measurement protocols require application of complex microwave pulse sequences of high precision and relatively high power, placing limitations on the design and scalability of these techniques. Here we demonstrate a microwave-free method for nanoscale NMR using the NV centre, which is a far less invasive, and vastly simpler measurement protocol. By utilising a carefully tuned magnetic cross-relaxation interaction between a subsurface NV spin and an external, organic environment of proton spins, we demonstrate NMR spectroscopy of $^1$H within a $\approx(10~{\rm nm})^3$ sensing volume. We also theoretically and experimentally show that the sensitivity of our approach matches that of existing microwave control-based techniques using the NV centre. Removing the requirement for coherent manipulation of either the NV or the environmental spin quantum states represents a significant step towards the development of robust, non-invasive nanoscale NMR probes.

cond-mat.mes-hall↗

arXiv2016

Spin dynamics of diamond nitrogen-vacancy centres at the ground state level anti-crossing and all-optical low frequency magnetic field sensing

We investigate the photo-induced spin dynamics of single nitrogen-vacancy (NV) centres in diamond near the electronic ground state level anti-crossing (GSLAC), which occurs at an axial magnetic field around 1024 G. Using optically detected magnetic resonance spectroscopy, we first find that the electron spin transition frequency can be tuned down to 100 kHz for the \NV{14} centre, while for the \NV{15} centre the transition strength vanishes for frequencies below about 2 MHz owing to the GSLAC level structure. Using optical pulses to prepare and readout the spin state, we observe coherent spin oscillations at 1024 G for the \NV{14}, which originate from spin mixing induced by residual transverse magnetic fields. This effect is responsible for limiting the smallest observable transition frequency, which can span two orders of magnitude from 100 kHz to tens of MHz depending on the local magnetic noise. A similar feature is observed for the \NV{15} centre at 1024 G. As an application of these findings, we demonstrate all-optical detection and spectroscopy of externally-generated fluctuating magnetic fields at frequencies from 8 MHz down to 500 kHz, using a \NV{14} centre. Since the Larmor frequency of most nuclear spin species lies within this frequency range near the GSLAC, these results pave the way towards all-optical, nanoscale nuclear magnetic resonance spectroscopy, using longitudinal spin cross-relaxation.

cond-mat.mes-hall↗

arXiv2016

Wide-band, nanoscale magnetic resonance spectroscopy using quantum relaxation of a single spin in diamond

We demonstrate a wide-band all-optical method of nanoscale magnetic resonance (MR) spectroscopy under ambient conditions. Our method relies on cross-relaxation between a probe spin, the electronic spin of a nitrogen-vacancy centre in diamond, and target spins as the two systems are tuned into resonance. By optically monitoring the spin relaxation time ($T_1$) of the probe spin while varying the amplitude of an applied static magnetic field, a frequency spectrum of the target spin resonances, a $T_1$-MR spectrum, is obtained. As a proof of concept, we measure $T_1$-MR spectra of a small ensemble of $^{14}$N impurities surrounding the probe spin within the diamond, with each impurity comprising an electron spin 1/2 and a nuclear spin 1. The intrinsically large bandwidth of the technique and probe properties allows us to detect both electron spin transitions -- in the GHz range -- and nuclear spin transitions -- in the MHz range -- of the $^{14}$N spin targets. The measured frequencies are found to be in excellent agreement with theoretical expectations, and allow us to infer the hyperfine, quadrupole and gyromagnetic constants of the target spins. Analysis of the strength of the resonances obtained in the $T_1$-MR spectrum reveals that the electron spin transitions are probed via dipole interactions, while the nuclear spin resonances are dramatically enhanced by hyperfine coupling and an electron-mediated process. Finally, we investigate theoretically the possibility of performing $T_1$-MR spectroscopy on nuclear spins without hyperfine interaction and predict single-proton sensitivity using current technology. This work establishes $T_1$-MR as a simple yet powerful technique for nanoscale MR spectroscopy, with broadband capability and a projected sensitivity down to the single nuclear spin level.

quant-ph↗

arXiv2015

Magneto-optical imaging of thin magnetic films using spins in diamond

Imaging the fields of magnetic materials provides crucial insight into the physical and chemical processes surrounding magnetism, and has been a key ingredient in the spectacular development of magnetic data storage. Existing approaches using the magneto-optic Kerr effect (MOKE), x-ray and electron microscopy have limitations that constrain further development, and there is increasing demand for imaging and characterisation of magnetic phenomena in real time with high spatial resolution. In this work, we show how the magneto-optical response of an array of negatively-charged nitrogen-vacancy spins in diamond can be used to image and map the sub-micron stray magnetic field patterns from thin ferromagnetic films. Using optically detected magnetic resonance, we demonstrate wide-field magnetic imaging over 100x100 μm^2 with a diffraction-limited spatial resolution of 440 nm at video frame rates, under ambient conditions. We demonstrate a novel all-optical spin relaxation contrast imaging approach which can image magnetic structures in the absence of an applied microwave field. Straightforward extensions promise imaging with sub-μT sensitivity and sub-optical spatial and millisecond temporal resolution. This work establishes practical diamond-based wide-field microscopy for rapid high-sensitivity characterisation and imaging of magnetic samples, with the capability for investigating magnetic phenomena such as domain wall and skyrmion dynamics and the spin Hall effect in metals.

cond-mat.mes-hall↗

arXiv2013

Analytic solutions to the central spin problem for Nitrogen Vacancy centres in diamond

Due to interest in both solid state based quantum computing architectures and the application of quantum mechanical systems to nanomagnetometry, there has been considerable recent attention focused on understanding the microscopic dynamics of solid state spin baths and their effects on the coherence of a controllable, coupled central electronic spin. Many analytic approaches are based on simplified phenomenological models in which it is difficult to capture much of the complex physics associated with this system. Conversely, numerical approaches reproduce this complex behaviour, but are limited in the amount of theoretical insight they can provide. Using a systematic approach based on the spatial statistics of spin bath constituents, we develop a purely analytic theory for the central spin decoherence problem of Nitrogen Vacancy centres in diamond that reproduces the experimental and numerical results found in the literature, whilst correcting a number of limitations and inaccuracies associated with existing analytical approaches.

cond-mat.mes-hall↗

arXiv2013

Single molecule NMR detection and spectroscopy using single spins in diamond

Nanomagnetometry using the nitrogen-vacancy (NV) centre in diamond has attracted a great deal of interest because of the combined features of room temperature operation, nanoscale resolution and high sensitivity. One of the important goals for nano-magnetometry is to be able to detect nanoscale nuclear magnetic resonance (NMR) in individual molecules. Our theoretical analysis shows how a single molecule at the surface of diamond, with characteristic NMR frequencies, can be detected using a proximate NV centre on a time scale of order seconds with nanometer precision. We perform spatio-temporal resolution optimisation and also outline paths to greater sensitivity. In addition, the method is suitable for application in low and relatively inhomogeneous background magnetic fields in contrast to both conventional liquid and solid state NMR spectroscopy.

quant-ph↗

arXiv2013

Detection of atomic spin labels in a lipid bi-layer using a single-spin nanodiamond probe

Magnetic field fluctuations arising from fundamental spins are ubiquitous in nanoscale biology, and are a rich source of information about the processes that generate them. However, the ability to detect the few spins involved without averaging over large ensembles has remained elusive. Here we demonstrate the detection of gadolinium spin labels in an artificial cell membrane under ambient conditions using a single-spin nanodiamond sensor. Changes in the spin relaxation time of the sensor located in the lipid bilayer were optically detected and found to be sensitive to near-individual proximal gadolinium atomic labels. The detection of such small numbers of spins in a model biological setting, with projected detection times of one second, opens a new pathway for in-situ nanoscale detection of dynamical processes in biology.

physics.bio-ph↗

arXiv2010

Dynamical Decoupling of a single electron spin at room temperature

Here we report the increase of the coherence time T$_2$ of a single electron spin at room temperature by using dynamical decoupling. We show that the Carr-Purcell-Meiboom-Gill (CPMG) pulse sequence can prolong the T$_2$ of a single Nitrogen-Vacancy center in diamond up to 2.44 ms compared to the Hahn echo measurement where T$_2 = 390 μ$s. Moreover, by performing spin locking experiments we demonstrate that with CPMG the maximum possible $T_2$ is reached. On the other hand, we do not observe strong increase of the coherence time in nanodiamonds, possibly due to the short spin lattice relaxation time $T_1=100 μ$s (compared to T$_1$ = 5.93 ms in bulk). An application for detecting low magnetic field is demonstrated, where we show that the sensitivity using the CPMG method is improved by about a factor of two compared to the Hahn echo method.

quant-ph↗

arXiv2010

Ultra-sensitive Diamond Magnetometry Using Optimal Dynamic Decoupling

New magnetometry techniques based on Nitrogen Vacancy (NV) defects in diamond have received much attention of late as a means to probe nanoscale magnetic environments. The sensitivity of a single NV magnetometer is primarily determined by the transverse spin relaxation time, $T_2$. Current approaches to improving the sensitivity employ crystals with a high NV density at the cost of spatial resolution, or extend $T_2$ via the manufacture of novel isotopically pure diamond crystals. We adopt a complementary approach, in which optimal dynamic decoupling techniques extend coherence times out to the self-correlation time of the spin bath. This suggests single spin, room temperature magnetometer sensitivities as low as 5\,pT\,Hz$^{-1/2}$ with current technology.

quant-ph↗

arXiv2009

Sensing of Fluctuating Nanoscale Magnetic Fields Using NV Centres in Diamond

New magnetometry techniques based on Nitrogen-Vacancy (NV) defects in diamond allow for the imaging of static (DC) and oscillatory (AC) nanoscopic magnetic systems. However, these techniques require accurate knowledge and control of the sample dynamics, and are thus limited in their ability to image fields arising from rapidly fluctuating (FC) environments. We show here that FC fields place restrictions on the DC field sensitivity of an NV qubit magnetometer, and that by probing the dephasing rate of the qubit in a magnetic FC environment, we are able to measure fluctuation rates and RMS field strengths that would be otherwise inaccessible with the use of DC and AC magnetometry techniques. FC sensitivities are shown to be comparable to those of AC fields, whilst requiring no additional experimental overheads or control over the sample.

cond-mat.mes-hall↗