As a complementary analysis tool to conventional high-field NMR, zero- to ultralow-field (ZULF) NMR detects nuclear magnetization signals in the sub-microtesla regime. Spin-exchange relaxation-free (SERF) atomic magnetometers provide a new generation of sensitive detector for ZULF NMR. Due to the features such as low-cost, high-resolution and potability, ZULF NMR has recently attracted considerable attention in chemistry, biology, medicine, and tests of fundamental physics. This review describes the basic principles, methodology and recent experimental and theoretical development of ZULF NMR, as well as its applications in spectroscopy, quantum control, imaging, NMR-based quantum devices, and tests of fundamental physics. The future prospects of ZULF NMR are also discussed.
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