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Free-electron lasers (FELs) are the world's most brilliant light sources with rapidly evolving technological capabilities in terms of ultrabright and ultrashort pulses over a large range of photon energies. Their revolutionary and innovative developments have opened new fields of science regarding nonlinear light-matter interaction, the investigation of ultrafast processes from specific observer sites, and approaches to imaging matter with atomic resolution. A core aspect of FEL science is the study of isolated and prototypical systems in the gas phase with the possibility of addressing well-defined electronic transitions or particular atomic sites in molecules. Notably for polarization-controlled short-wavelength FELs, the gas phase offers new avenues for investigations of nonlinear and ultrafast phenomena in spin-orientated systems, for decoding the function of the chiral building blocks of life as well as steering reactions and particle emission dynamics in otherwise inaccessible ways. This roadmap comprises descriptions of technological capabilities of facilities worldwide, innovative diagnostics and instrumentation, as well as recent scientific highlights, novel methodology, and mathematical modeling. The experimental and theoretical landscape of using polarization controllable FELs for dichroic light-matter interaction in the gas phase will be discussed and comprehensively outlined to stimulate and strengthen global collaborative efforts of all disciplines. Published by the American Physical Society2025 

Observation of lasing signals at multiple wavelengths in argon atoms pumped by a 3-photon resonance with an intense 260 nm laser were used to observe the dynamics of electronic excited states. 

Absolute density measurements of low-ionization-degree or low-density plasmas ionized by lasers are very important for understanding strong-field physics, atmospheric propagation of intense laser pulses, Lidar etc. A cross-polarized common-path temporal interferometer using balanced detection was developed for measuring plasma density with a sensitivity of ∼0.6 mrad, equivalent to a plasma density-length product of ∼2.6 × 10¹³cm⁻²if using an 800 nm probe laser. By using this interferometer, we have investigated strong-field ionization yield versus intensity for various noble gases (Ar, Kr, and Xe) using 800 nm, 55 fs laser pulses with both linear (LP) and circular (CP) polarization. The experimental results were compared to the theoretical models of Ammosov-Delone-Krainov (ADK) and Perelomov-Popov-Terent’ev (PPT). We find that the measured phase change induced by plasma formation can be explained by the ADK theory in the adiabatic tunneling ionization regime, while PPT model can be applied to all different regimes. We have also measured the photoionization and fractional photodissociation of molecular (MO) hydrogen. By comparing our experimental results with PPT and MO-PPT models, we have determined the likely ionization pathways when using three different pump laser wavelengths of 800 nm, 400 nm, and 267 nm.