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High resolution two-photon spectroscopy of ¹²⁹Xe for precision optical magnetometry Altiere, Emily


This dissertation presents high precision two-photon xenon spectroscopy of the 5p₅(²P₃/₂)6p²[3/2]₂ ⟵5p⁶(¹S₀) transition. Specific attention is paid to the F = 3/2 hyperfine level of ¹²⁹Xe, motivated by the new experiment at TRIUMF to measure the electric dipole moment of the neutron. A non-zero value of the nEDM would partially confirm the existence of the baryon asymmetry in the universe as predicted by theories beyond the standard model. To achieve this measurement, ¹²⁹Xe is proposed for use in a cohabiting ¹⁹⁹Hg/¹²⁹Xe optical comagnetometer. To date, no laser system has existed to probe the specific xenon transition required for this measurement. We developed a novel continuous-wave 252.4 nm ultra-violet (UV) laser system with the power and precision to selectively probe the hyperfine levels of ¹²⁹Xe. Using this laser, we observed the first high resolution two-photon transition spectrum of xenon, which is comprised of ten transition peaks across the six most abundant isotopes, including the hyperfine levels of the ¹²⁹Xe and ¹³¹Xe. Detailed analysis of this spectrum revealed the hyperfine constants of the 5p₅(²P₃/₂)6p²[3/2]₂ excited state and other constants relating to the isotope shift. Furthermore, we describe initial observations into the pressure dependencies of the spectral lineshape from 15–980 mTorr. The ¹²⁹Xe pressure in the nEDM experiment is limited to 3 mTorr, making it essential to characterize the xenon signal at low pressures to maximize comagnetometer sensitivity. Intriguingly, our results suggest that ¹²⁹Xe qualitatively exhibits nonlinear pressure broadening at low pressure (

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