Intensity-dependent precision two-photon Doppler-free spectroscopy of Xe using narrow-bandwidth long-pulse deep-UV laser radiation

Abstract

We report on a precision measurement of the $(5\mathrm{p})^{5}6\mathrm{p} \, [1/2]_{0}\leftarrow (5\mathrm{p})^{6} \, ^{1}\mathrm{S}_{0}$ transition wavenumber of Xe by Doppler-free two-photon spectroscopy using near-Fourier-transform-limited long pulses of UV-laser radiation. The measurements led to absolute uncertainties of 750~kHz in the two-photon transition wavenumbers for the five dominant isotopes of Xe, e.g., 80118.982918(27)~cm$^{-1}$ for $^{136}$Xe. These values were combined with other precision measurements in Xe to resolve an $\sim1~\mathrm{GHz}$ discrepancy between the ionization energy of Xe obtained in recent measurements from the $(6{\rm s})[3/2]_2$ metastable state [Herburger {\it et al.} Phys. Rev. A {\bf 109}, 032816 (2024)] and the ionization energy listed in the NIST atomic database. The analysis indicates that the natural-abundance-weighted ionization energy of Xe should be revised by $-0.023$~cm$^{-1}$ to 97833.7641(20)~cm$^{-1}$. Large fluctuations in the UV-laser pulse intensities were exploited to characterize intensity-dependent shifts of the observed two-photon transition frequencies. Shifts of up to $- 20~\mathrm{MHz}$ were observed and attributed to frequency shifts arising from chirps in the amplification and upconversion of the laser radiation rather than to the ac-Stark effect.