We present single- and multiple-quantum correlation J-spectroscopy detected in zero (<1μG) magnetic field using a ⁸⁷Rb vapor-cell magnetometer. At zero field the spectrum of ethanol appears as a mixture of ¹³C isotopomers, and correlation spectroscopy is useful in separating the two composite spectra. We also identify and observe the zero-field equivalent of a double-quantum transition in ¹³C₂-acetic acid, and show that such transitions are of use in spectral assignment. Two-dimensional spectroscopy further improves the high resolution attained in zero-field NMR since selection rules on the coherence-transfer pathways allow for the separation of otherwise overlapping resonances into distinct cross-peaks.

We use a radio-frequency 85Rb alkali-vapor cell magnetometer based on a paraffin-coated cell with long spin-coherence time and a small, low-inductance driving coil to create highly resolved conductivity maps of different objects. We resolve sub-mm features in conductive objects, we characterize the frequency response of our technique, and by operating at frequencies up to 250 kHz we are able to discriminate between differently conductive materials based on the induced response. The method is suited to cover a wide range of driving frequencies and can potentially be used for detecting non-metallic objects with low DC conductivity.

We review instrumentation for nuclear magnetic resonance (NMR) in zero and ultra-low magnetic field (ZULF, below 0.1 $\mu$T) where detection is based on a low-cost, non-cryogenic, spin-exchange relaxation free (SERF) $^{87}$Rb atomic magnetometer. The typical sensitivity is 20-30 fT/Hz$^{1/2}$ for signal frequencies below 1 kHz and NMR linewidths range from Hz all the way down to tens of mHz. These features enable precision measurements of chemically informative nuclear spin-spin couplings as well as nuclear spin precession in ultra-low magnetic fields.

We report observation of long-lived spin-singlet states in a 13C-1H spin pair at zero magnetic field. In 13C-labeled formic acid, we observe spin-singlet lifetimes as long as 37 seconds, about a factor of three longer than the T1 lifetime of dipole polarization in the triplet state. We also observe that the lifetime of the singlet-triplet coherence, T2, is longer than T1. Moreover, we demonstrate that this singlet states formed by spins of a heteronucleus and a 1H nucleus, can exhibit longer lifetimes than the respective triplet states in systems consisting of more than two nuclear spins. Although long-lived homonuclear spin-singlet states have been extensively studied, this is the first experimental observation of analogous spin-singlets consisting of a heteronucleus and a proton.

Hyperpolarized fumarate is a promising biosensor for carbon-13 magnetic resonance metabolic imaging. Such molecular imaging applications require nuclear hyperpolarization to attain sufficient signal strength. Dissolution dynamic nuclear polarization is the current state-of-the-art methodology for hyperpolarizing fumarate, but this is expensive and relatively slow. Alternatively, this important biomolecule can be hyperpolarized in a cheap and convenient manner using parahydrogen-induced polarization. However, this process requires a chemical reaction, and the resulting solutions are contaminated with the catalyst, unreacted reagents, and reaction side-product molecules, and are hence unsuitable for use in vivo. In this work we show that the hyperpolarized fumarate can be purified from these contaminants by acid precipitation as a pure solid, and later redissolved to a desired concentration in a clean aqueous solvent. Significant advances in the reaction conditions and reactor equipment allow for formation of hyperpolarized fumarate at 13C polarization levels of 30-45%.

Zero- to ultralow-field (ZULF) nuclear magnetic resonance (NMR) is an emerging tool for precision chemical analysis. In this work, we study dynamic processes and investigate the influence of chemical exchange on ZULF NMR J-spectra. We develop a computational approach that allows quantitative calculation of J-spectra in the presence of chemical exchange and apply it to study aqueous solutions of [¹⁵N]ammonium (¹⁵N[Formula: see text]) as a model system. We show that pH-dependent chemical exchange substantially affects the J-spectra and, in some cases, can lead to degradation and complete disappearance of the spectral features. To demonstrate potential applications of ZULF NMR for chemistry and biomedicine, we show a ZULF NMR spectrum of [2-¹³C]pyruvic acid hyperpolarized via dissolution dynamic nuclear polarization (dDNP). We foresee applications of affordable and scalable ZULF NMR coupled with hyperpolarization to study chemical exchange phenomena in vivo and in situations where high-field NMR detection is not possible to implement.