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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 

Abstract Resonant oscillators with stable frequencies and large quality factors help us to keep track of time with high precision. Examples range from quartz crystal oscillators in wristwatches to atomic oscillators in atomic clocks, which are, at present, our most precise time measurement devices¹. The search for more stable and convenient reference oscillators is continuing^2–6. Nuclear oscillators are better than atomic oscillators because of their naturally higher quality factors and higher resilience against external perturbations^7–9. One of the most promising cases is an ultra-narrow nuclear resonance transition in⁴⁵Sc between the ground state and the 12.4-keV isomeric state with a long lifetime of 0.47 s (ref. ¹⁰). The scientific potential of⁴⁵Sc was realized long ago, but applications require⁴⁵Sc resonant excitation, which in turn requires accelerator-driven, high-brightness X-ray sources¹¹that have become available only recently. Here we report on resonant X-ray excitation of the⁴⁵Sc isomeric state by irradiation of Sc-metal foil with 12.4-keV photon pulses from a state-of-the-art X-ray free-electron laser and subsequent detection of nuclear decay products. Simultaneously, the transition energy was determined as$${\mathrm{12,389.59}}_{+0.12\left({\rm{syst}}\right)}^{\pm 0.15\left({\rm{stat}}\right)}\,{\rm{eV}}$$ ${\mathrm{12,389.59}}_{+0.12\left(\mathrm{syst}\right)}^{\pm 0.15\left(\mathrm{stat}\right)}\mathrm{eV}$with an uncertainty that is two orders of magnitude smaller than the previously known values. These advancements enable the application of this isomer in extreme metrology, nuclear clock technology, ultra-high-precision spectroscopy and similar applications.