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Register a new userPreparation of Nuclear Spin Singlet States using Spin-Lock Induced Crossing
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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 D2O, 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 timescale as spin-lattice relaxation.
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Nuclear magnetic resonance (NMR) spectroscopy usually requires high magnetic fields to create spectral resolution among different proton species. At low fields, chemical shift dispersion is insufficient to separate the species, and the spectrum exhibits just a single line. In this work, we demonstrate that spectra can nevertheless be acquired at low field using a novel pulse sequence called spin-lock induced crossing (SLIC). This probes energy level crossings induced by a weak spin-locking pulse and produces a unique J-coupling spectrum for most organic molecules. Unlike other forms of low-field J-coupling spectroscopy, our technique does not require the presence of heteronuclei and can be used for most compounds in their native state. We performed SLIC spectroscopy on a number of small molecules at 276 kHz and 20.8 MHZ, and we show that SLIC spectra can be simulated in good agreement with measurements.
The coherent high-fidelity generation of nuclear spins in long-lived singlet states which may find application as quantum memory or sensor represents a considerable experimental challenge. Here we propose a dissipative scheme that achieves the preparation of pairs of nuclear spins in long-lived singlet states by a protocol that combines the interaction between the nuclei and a periodically reset electron spin of an NV center with local rf-control of the nuclear spins. The final state of this protocol is independent of the initial preparation of the nuclei, is robust to external field fluctuations and can be operated at room temperature. We show that a high fidelity singlet pair of a 13C dimer in a nuclear bath in diamond can be generated under realistic experimental conditions.
$^{31}$P NMR and MRI are commonly used to study organophosphates that are central to cellular energy metabolism. In some molecules of interest, such as adenosine diphosphate (ADP) and nicotinamide adenine dinucleotide (NAD), pairs of coupled $^{31}$P nuclei in the diphosphate moiety should enable the creation of nuclear spin singlet states, which may be long-lived and can be selectively detected via quantum filters. Here, we show that $^{31}$P singlet states can be created on ADP and NAD, but their lifetimes are shorter than T$_{1}$ and are strongly sensitive to pH. Nevertheless, the singlet states were used with a quantum filter to successfully isolate the $^{31}$P NMR spectra of those molecules from the adenosine triphosphate (ATP) background signal.
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.
The generation and control of neutron orbital angular momentum (OAM) states and spin correlated OAM (spin-orbit) states provides a powerful probe of materials with unique penetrating abilities and magnetic sensitivity. We describe techniques to prepare and characterize neutron spin-orbit states, and provide a quantitative comparison to known procedures. The proposed detection method directly measures the correlations of spin state and transverse momentum, and overcomes the major challenges associated with neutrons, which are low flux and small spatial coherence length. Our preparation techniques, utilizing special geometries of magnetic fields, are based on coherent averaging and spatial control methods borrowed from nuclear magnetic resonance. The described procedures may be extended to other probes such as electrons and electromagnetic waves.
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