Quadrature-detected zero-to-ultralow-field nuclear magnetic resonance

We present the concept of quadrature-detected zero-to-ultralow-field nuclear magnetic resonance (QD ZULF NMR). Two orthogonal sensors, atomic optically pumped magnetometers, are used to separately detect components of oscillating sample magnetization, which are then combined into a quadrature signal. This approach enables the distinction of positive and negative resonance frequencies with respect to the laboratory frame---such that absolute signs of gyromagnetic ratios can be determined. In addition, QD ZULF NMR reduces peak density and overlap compared to ZULF NMR with single-axis detection, while providing richer information about nuclear-spin dynamics. As an illustration, we present experimental J-spectra for thermally polarized [13 C]-formic acid and [13 C]-methanol, compounds commonly used in ZULF NMR which represent XA and XA 3 spin systems, respectively. A theoretical framework describing QD ZULF NMR signals is provided.