Non-linear self-driven spectral tuning of Extreme Ultraviolet Femtosecond Pulses in monoatomic materials

Self-action nonlinearity is a key aspect - either as a foundational element or a detrimental factor - of several optical spectroscopies and photonic devices. Supercontinuum generation, wavelength converters, and chirped pulse amplification are just a few examples. The recent advent of Free Electron Lasers (FEL) fostered building on nonlinearity to propose new concepts and extend optical wavelengths paradigms for extreme ultraviolet (EUV) and X-ray regimes. No evidence for intrapulse dynamics, however, has been reported at such short wavelengths, where the light-matter interactions are ruled by the sharp absorption edges of core electrons. Here, we provide experimental evidence for self-phase modulation of femtosecond FEL pulses, which we exploit for fine self-driven spectral tunability by interaction with sub-micrometric foils of selected monoatomic materials. Moving the pulse wavelength across the absorption edge, the spectral profile changes from a non-linear spectral blue-shift to a red-shifted broadening. These findings are rationalized accounting for ultrafast ionization and delayed thermal response of highly excited electrons above and below threshold, respectively.

Automated summary

Self-action nonlinearity plays a crucial role in various optical spectroscopies and photonic devices, with recent advancements in Free Electron Lasers (FEL) offering new opportunities to extend optical wavelength paradigms. Experimental evidence shows that femtosecond FEL pulses can be self-phase modulated for spectral tunability, with potential applications in extreme ultraviolet and X-ray regimes. The findings are rationalized by considering ultrafast ionization and delayed thermal response of highly excited electrons above and below threshold.