Imaging-assisted single-photon Doppler-free laser spectroscopy and the ionization energy of metastable triplet helium

TL;DR

This paper introduces an imaging method to eliminate Doppler broadening in laser spectroscopy of metastable helium, achieving near-atomic resolution and accurately determining the ionization energy, resolving previous experimental-theoretical discrepancies.

Contribution

The authors develop a novel imaging technique that suppresses residual Doppler broadening, enabling high-resolution spectra and precise ionization energy measurement of metastable helium.

Findings

Doppler broadening reduced to about 1 MHz in UV spectra.

Successful determination of the ionization energy of metastable triplet helium.

Confirmed discrepancy between recent experimental and theoretical ionization energies.

Abstract

Skimmed supersonic beams provide intense, cold, collision-free samples of atoms and molecules are one of the most widely used tools in atomic and molecular laser spectroscopy. High-resolution optical spectra are typically recorded in a perpendicular arrangement of laser and supersonic beams to minimize Doppler broadening. Typical Doppler widths are nevertheless limited to tens of MHz by the residual transverse-velocity distribution in the gas-expansion cones. We present an imaging method to overcome this limitation which exploits the correlation between the positions of the atoms and molecules in the supersonic expansion and their transverse velocities - and thus their Doppler shifts. With the example of spectra of $(1\mathrm{s})(n\mathrm{p})\,^3\mathrm{P}_{0-2}\leftarrow (1\mathrm{s})(2\mathrm{s})\,^3\mathrm{S}_1$ transitions to high Rydberg states of metastable triplet He, we demonstrate the suppression of the residual Doppler broadening and a reduction of the full linewidths at half maximum to only about 1 MHz in the UV. Using a retro-reflection arrangement for the laser beam and a cross-correlation method, we determine Doppler-free spectra without any signal loss from the selection, by imaging, of atoms within ultranarrow transverse-velocity classes. As an illustration, we determine the ionization energy of triplet metastable He and confirm the significant discrepancy between recent experimental (Clausen et al., Phys. Rev. Lett. 127 093001 (2021)) and high-level theoretical (Patk\'os et al., Phys. Rev. A 103 042809 (2021)) values of this quantity.