Optically pumped magnetometers (OPMs) based on alkali-atom vapors are ultra-sensitive devices for dc and low-frequency ac magnetic measurements. Here, in combination with fast-field-cycling hardware and high-resolution spectroscopic detection, we demonstrate applicability of OPMs in quantifying nuclear magnetic relaxation phenomena. Relaxation rate dispersion across the nT to mT field range enables quantitative investigation of extremely slow molecular motion correlations in the liquid state, with time constants > 1 ms, and insight into the corresponding relaxation mechanisms. The 10-20 fT/$$\sqrt{{\rm{H}}}{\rm{z}}$$ H z sensitivity of an OPM between 10 Hz and 5.5 kHz 1H Larmor frequency suffices to detect magnetic resonance signals from ~ 0.1 mL liquid volumes imbibed in simple mesoporous materials, or inside metal tubing, following nuclear spin prepolarization adjacent to the OPM. High-resolution spectroscopic detection can resolve inter-nucleus spin-spin couplings, further widening the scope of application to chemical systems. Expected limits of the technique regarding measurement of relaxation rates above 100 s−1 are discussed.
The individual and coherent control of solid-state based electron spins is important covering fields from quantum information processing and quantum metrology to material research and medical imaging. Especially for the control of individual spins in nanoscale networks, the generation of strong, fast, and localized magnetic fields is crucial. Highly engineered devices that demonstrate most of the desired features are found in nanometer size magnetic writers of hard disk drives (HDD). Currently, however, their nanoscale operation in particular comes at the cost of excessive magnetic noise. Here, we present HDD writers as a tool for the efficient manipulation of single as well as multiple spins. We show that their tunable gradients of up to 100 μT/nm can be used to spectrally address individual spins on the nanoscale. Their gigahertz bandwidth allows one to switch control fields within nanoseconds, faster than characteristic time scales such as Rabi and Larmor periods, spin-spin couplings, or optical transitions, thus extending the set of feasible spin manipulations. We used the fields to drive spin transitions through nonadiabatic fast passages or to enable the optical readout of spin states in strong misaligned fields. Building on these techniques, we further apply the large magnetic field gradients for microwave selective addressing of single spins and show its use for the nanoscale optical colocalization of two emitters.
We demonstrate a method to quantify and manipulate nuclear spin decoherence mechanisms that are active in zero to ultralow magnetic fields. These include (i) nonadiabatic switching of spin quantization axis due to residual background fields and (ii) scalar pathways due to through-bond couplings between 1H and heteronuclear spin species, such as 2H used partially as an isotopic substitute for 1H. Under conditions of free evolution, scalar relaxation due to 2H can significantly limit nuclear spin polarization lifetimes and thus the scope of magnetic resonance procedures near zero field. It is shown that robust trains of pulsed dc magnetic fields that apply π flip angles to one or multiple spin species may switch the effective symmetry of the nuclear spin Hamiltonian, imposing decoupled or coupled dynamic regimes on demand. The method should broaden the spectrum of hyperpolarized biomedical contrast-agent compounds and hyperpolarization procedures that are used near zero field.
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