Demonstration of Ramsey-Comb Precision Spectroscopy in Xenon at Vacuum Ultraviolet Wavelengths Produced with High-Harmonic Generation

TL;DR

This paper demonstrates the use of Ramsey-comb spectroscopy in xenon at vacuum ultraviolet wavelengths generated by high-harmonic generation, achieving sub-MHz precision and significantly improving measurement accuracy of atomic transitions.

Contribution

It introduces a novel application of Ramsey-comb spectroscopy to VUV wavelengths, enabling high-precision measurements in xenon with reduced phase shifts from HHG.

Findings

Achieved sub-MHz accuracy in xenon transition frequency measurement.

Reduced phase shifts from HHG to negligible levels, enabling precise spectroscopy.

Improved the precision of isotope shift measurements between xenon isotopes.

Abstract

The remarkable progress in the field of laser spectroscopy induced by the invention of the frequency-comb laser has enabled many new high-precision tests of fundamental theory and searches for new physics. Extending frequency-comb based spectroscopy techniques to the vacuum (VUV) and extreme ultraviolet (XUV) spectral range would enable measurements in e.g. heavier hydrogen-like systems and open up new possibilities for tests of quantum electrodynamics and measurements of fundamental constants. The main approaches rely on high-harmonic generation (HHG), which is known to induce spurious phase shifts from plasma formation. After our initial report (Physical Review Letters 123, 143001 (2019)), we give a detailed account of how the Ramsey-comb technique is used to probe the plasma dynamics with high precision, and enables accurate spectroscopy in the VUV. A series of Ramsey fringes is recorded to track the phase evolution of a superposition state in xenon atoms, excited by two up-converted frequency-comb pulses. Phase shifts of up to 1 rad induced by HHG were observed at ns timescales and with mrad-level accuracy at $110$ nm. Such phase shifts could be reduced to a negligible level, enabling us to measure the $5p^6 \rightarrow 5p^5 8s~^2[3/2]_1$ transition frequency in $^{132}Xe$ at 110 nm (seventh harmonic) with sub-MHz accuracy. The obtained value is $10^4$ times more precise than the previous determination and the fractional accuracy of $2.3 \times 10^{-10}$ is $3.6$ times better than the previous best spectroscopic measurement using HHG. The isotope shifts between $^{132}Xe$ and two other isotopes were determined with an accuracy of $420$ kHz. The method can be readily extended to achieve kHz-level accuracy, e.g. to measure the $1S-2S$ transition in $He^+$. Therefore, the Ramsey-comb method shows great promise for high-precision spectroscopy of targets requiring VUV and XUV wavelengths.