# Vacuum-ultraviolet frequency-modulation spectroscopy

## TL;DR

This paper extends frequency-modulation spectroscopy to the vacuum-ultraviolet range, enabling sensitive, background-free VUV absorption measurements using table-top lasers and demonstrating its effectiveness on noble gases and nitrogen.

## Contribution

The authors develop a novel VUV FM spectroscopy method using resonance-enhanced sum-frequency mixing and demonstrate its advantages over traditional techniques.

## Key findings

- High sensitivity and background-free VUV spectra obtained
- Simultaneous recording of absorption, fluorescence, and photoionization spectra
- Effective for cold samples in supersonic beams

## Abstract

Frequency-modulation (FM) spectroscopy has been extended to the vacuum-ultraviolet (VUV) range of the electromagnetic spectrum. Coherent VUV laser radiation is produced by resonance-enhanced sum-frequency mixing ($\nu_{\mathrm{VUV}}=2\nu_{\mathrm{UV}}+\nu_2$) in Kr and Xe using two near-Fourier-transform-limited laser pulses of frequencies $\nu_{\mathrm{UV}}$ and $\nu_2$. Sidebands generated in the output of the second laser ($\nu_2$) using an electro-optical modulator operating at the frequency $\nu_{\mathrm{mod}}$ are directly transfered to the VUV and used to record FM spectra. Demodulation is demonstrated both at $\nu_{\mathrm{mod}}$ and $2\nu_{\mathrm{mod}}$. The main advantages of the method are that its sensitivity is not reduced by pulse-to-pulse fluctuations of the VUV laser intensity, compared to VUV absorption spectroscopy is its background-free nature, the fact that its implementation using table-top laser equipment is straightforward and that it can be used to record VUV absorption spectra of cold samples in skimmed supersonic beams simultaneously with laser-induced-fluorescence and photoionization spectra. To illustrate these advantages we present VUV FM spectra of Ar, Kr, and N$_2$ in selected regions between 105000cm$^{-1}$ and 122000cm$^{-1}$.