Optical Magnetometry Using Multiphoton Transitions

Abstract

Optical magnetometry plays a critical role in low-energy precision measurements and numerous other applications. In particular, permanent electric dipole moment (EDM) searches impose strict requirements on magnetic field sensitivity of the underlying atomic or molecular species. Other magnetometer properties -- such as chemical reactivity, dielectric strength, and interaction cross-sections with other species -- also impose limitations on experimental conditions.

Here, we explore a novel approach to optical magnetometry, using multiphoton transitions of diamagnetic atoms to detect Larmor precession of polarized nuclei. Resonant probes are possible at moderate ultraviolet wavelengths, and hyperfine structure couples spin precession to fluorescence transitions with negligible backgrounds; paramagnetic rotation due to intensity-dependent dispersion may also be detectable. Nuclear spins and nonlinear optical excitation introduce new degrees of freedom, and evade limitations arising from rapid electronic decoherence.

This dissertation reports progress towards two-photon optical magnetometry using ytterbium, rubidium, and xenon. We characterize the influence of probe polarization and magnetic fields on fluorescence spectra, for one- and two-photon continuous-wave (cw) excitation of ytterbium. Resolved hyperfine and isotope structure allow us to use spin-zero isotopes for diagnostics and normalization, and we develop analysis for overlapping two-photon resonances. We also report measurements of two-photon excitation in ytterbium and rubidium using picosecond laser pulses, and in xenon using a cw laser. Although hyperfine structure is unresolved, the rubidium measurements are sensitive to probe field polarization. Fluorescence spectra from two-photon excitation of ytterbium with femtosecond pulses show modulation when the repetition rate changes.

Although techniques for polarizing noble gas nuclei are mature, existing cell designs are incompatible with two-photon magnetometry. We describe development of silicate-assisted hydroxide-catalysis bonding for both aluminosilicate EDM cells with silicon electrodes, and sapphire-windowed cells that transmit ultraviolet excitation light. Progress in measuring the 129Xe nuclear EDM is discussed. Absolute referencing of the picosecond laser to potassium transitions is proposed for two-photon spectroscopy of ytterbium and xenon, and a compatible frequency-tripling method is outlined to produce excitation light for xenon. Novel possibilities including spatial resolution and multiphoton optical pumping of nuclear spins are considered.