96 research outputs found
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Nuclear Magnetic Resonance with Spin Singlet States and Nitrogen Vacancy Centers in Diamond
Nuclear magnetic resonance (NMR) spectroscopy and magnetic resonance imaging (MRI) are techniques widely utilized by many scientific fields, but their applications are often limited by short spin relaxation times and low sensitivity. This thesis explores two novel forms of NMR addressing these issues: nuclear spin singlet states for extending spin polarization lifetime and nitrogen-vacancy centers for sensing small samples.Chemistry and Chemical Biolog
Dependence of nuclear spin singlet lifetimes on RF spin-locking power
We measure the lifetime of long-lived nuclear spin singlet states as a
function of the strength of the RF spin-locking field and present a simple
theoretical model that agrees well with our measurements, including the
low-RF-power regime. We also measure the lifetime of a long-lived coherence
between singlet and triplet states that does not require a spin-locking field
for preservation. Our results indicate that for many molecules, singlet states
can be created using weak RF spin-locking fields: more than two orders of
magnitude lower RF power than in previous studies. Our findings suggest that in
many biomolecules, singlets and related states with enhanced lifetimes might be
achievable in vivo with safe levels of RF power
Preparation of Nuclear Spin Singlet States Using Spin-Lock Induced Crossing
We introduce a broadly applicable technique to create nuclear spin singlet states in organic molecules and other many-atom systems. We employ a novel pulse sequence to produce a spin-lock induced crossing (SLIC) of the spin singlet and triplet energy levels, which enables triplet-singlet polarization transfer and singlet-state preparation. We demonstrate the utility of the SLIC method by producing a long-lived nuclear spin singlet state on two strongly coupled proton pairs in the tripeptide molecule phenylalanine-glycine-glycine dissolved in DO and by using SLIC to measure the J couplings, chemical shift differences, and singlet lifetimes of the proton pairs. We show that SLIC is more efficient at creating nearly equivalent nuclear spin singlet states than previous pulse sequence techniques, especially when triplet-singlet polarization transfer occurs on the same time scale as spin-lattice relaxation.Physic
A statistical learning framework for mapping indirect measurements of ergodic systems to emergent properties
The discovery of novel experimental techniques often lags behind contemporary
theoretical understanding. In particular, it can be difficult to establish
appropriate measurement protocols without analytic descriptions of the
underlying system-of-interest. Here we propose a statistical learning framework
that avoids the need for such descriptions for ergodic systems. We validate
this framework by using Monte Carlo simulation and deep neural networks to
learn a mapping between low-field nuclear magnetic resonance spectra and proton
exchange rates in ethanol-water mixtures. We found that trained networks
exhibited normalized-root-mean-square errors of less than 1% for exchange rates
under 150 s-1 but performed poorly for rates above this range. This
differential performance occurred because low-field measurements are
indistinguishable from one another at fast exchange. Nonetheless, where a
discoverable relationship between indirect measurements and emergent dynamics
exists, we demonstrate the possibility of approximating it without the need for
precise analytic descriptions, allowing experimental science to flourish in the
midst of ongoing theoretical wor
Fourier Magnetic Imaging with Nanoscale Resolution and Compressed Sensing Speed-up using Electronic Spins in Diamond
Optically-detected magnetic resonance using Nitrogen Vacancy (NV) color
centres in diamond is a leading modality for nanoscale magnetic field imaging,
as it provides single electron spin sensitivity, three-dimensional resolution
better than 1 nm, and applicability to a wide range of physical and biological
samples under ambient conditions. To date, however, NV-diamond magnetic imaging
has been performed using real space techniques, which are either limited by
optical diffraction to 250 nm resolution or require slow, point-by-point
scanning for nanoscale resolution, e.g., using an atomic force microscope,
magnetic tip, or super-resolution optical imaging. Here we introduce an
alternative technique of Fourier magnetic imaging using NV-diamond. In analogy
with conventional magnetic resonance imaging (MRI), we employ pulsed magnetic
field gradients to phase-encode spatial information on NV electronic spins in
wavenumber or k-space followed by a fast Fourier transform to yield real-space
images with nanoscale resolution, wide field-of-view (FOV), and compressed
sensing speed-up.Comment: 31 pages, 10 figure
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Optical magnetic imaging of living cells
Magnetic imaging is a powerful tool for probing biological and physical systems. However, existing techniques either have poor spatial resolution compared to optical microscopy and are hence not generally applicable to imaging of sub-cellular structure (e.g., magnetic resonance imaging [MRI]1), or entail operating conditions that preclude application to living biological samples while providing sub-micron resolution (e.g., scanning superconducting quantum interference device [SQUID] microscopy2, electron holography3, and magnetic resonance force microscopy [MRFM]4). Here we demonstrate magnetic imaging of living cells (magnetotactic bacteria) under ambient laboratory conditions and with sub-cellular spatial resolution (400 nm), using an optically-detected magnetic field imaging array consisting of a nanoscale layer of nitrogen-vacancy (NV) colour centres implanted at the surface of a diamond chip. With the bacteria placed on the diamond surface, we optically probe the NV quantum spin states and rapidly reconstruct images of the vector components of the magnetic field created by chains of magnetic nanoparticles (magnetosomes) produced in the bacteria, and spatially correlate these magnetic field maps with optical images acquired in the same apparatus. Wide-field sCMOS acquisition allows parallel optical and magnetic imaging of multiple cells in a population with sub-micron resolution and >100 micron field-of-view. Scanning electron microscope (SEM) images of the bacteria confirm that the correlated optical and magnetic images can be used to locate and characterize the magnetosomes in each bacterium. The results provide a new capability for imaging bio-magnetic structures in living cells under ambient conditions with high spatial resolution, and will enable the mapping of a wide range of magnetic signals within cells and cellular networks5, 6
Singlet NMR methodology in two-spin-1/2 systems
This paper discusses methodology developed over the past 12 years in order to access and manipulate singlet order in systems comprising two coupled spin-1/2 nuclei in liquid-state nuclear magnetic resonance. Pulse sequences that are valid for different regimes are discussed, and fully analytical proofs are given using different spin dynamics techniques that include product operator methods, the single transition operator formalism, and average Hamiltonian theory. Methods used to filter singlet order from byproducts of pulse sequences are also listed and discussed analytically. The theoretical maximum amplitudes of the transformations achieved by these techniques are reported, together with the results of numerical simulations performed using custom-built simulation code
Coherent evolution of parahydrogen induced polarisation using laser pump, NMR probe spectroscopy : Theoretical framework and experimental observation
We recently reported a pump-probe method that uses a single laser pulse to introduce parahydrogen (p-H2) into a metal dihydride complex and then follows the time-evolution of the p-H2-derived nuclear spin states by NMR. We present here a theoretical framework to describe the oscillatory behaviour of the resultant hyperpolarised NMR signals using a product operator formalism. We consider the cases where the p-H2-derived protons form part of an AX, AXY, AXYZ or AA′XX′ spin system in the product molecule. We use this framework to predict the patterns for 2D pump-probe NMR spectra, where the indirect dimension represents the evolution during the pump-probe delay and the positions of the cross-peaks depend on the difference in chemical shift of the p-H2-derived protons and the difference in their couplings to other nuclei. The evolution of the NMR signals of the p-H2-derived protons, as well as the transfer of hyperpolarisation to other NMR-active nuclei in the product, is described. The theoretical framework is tested experimentally for a set of ruthenium dihydride complexes representing the different spin systems. Theoretical predictions and experimental results agree to within experimental error for all features of the hyperpolarised 1H and 31P pump-probe NMR spectra. Thus we establish the laser pump, NMR probe approach as a robust way to directly observe and quantitatively analyse the coherent evolution of p-H2-derived spin order over micro-to-millisecond timescales
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