X-ray harmonics made with long-wavelength lasers reach higher fluxes and photon energies when plasma effects dominate.

Electron dynamics induced by resonant absorption of light is of fundamental importance in nature and has been the subject of countless studies in many scientific areas. Above the ionization threshold of atomic or molecular systems, the presence of discrete states leads to autoionization, which is an interference between two quantum paths: direct ionization and excitation of the discrete state coupled to the continuum. Traditionally studied with synchrotron radiation, the probability for autoionization exhibits a universal Fano intensity profile as a function of excitation energy. However, without additional phase information, the full temporal dynamics cannot be recovered. Here we use tunable attosecond pulses combined with weak infrared radiation in an interferometric setup to measure not only the intensity but also the phase variation of the photoionization amplitude across an autoionization resonance in argon. The phase variation can be used as a fingerprint of the interactions between the discrete state and the ionization continua, indicating a new route towards monitoring electron correlations in time.

Nitrogen molecules in ambient air exposed to an intense near-infrared femtosecond laser pulse give rise to cavity-free superradiant emission at 391.4 and 427.8 nm. An unexpected pulse duration-dependent cyclic variation of the superradiance intensity is observed when the central wavelength of the femtosecond pump laser pulse is finely tuned between 780 and 820 nm, and no signal occurs at the resonant wavelength of 782.8 nm ($2{\omega }_{782.8\mathrm{nm}}={\omega }_{391.4\mathrm{nm}}$). On the basis of a semiclassical recollision model, we show that an interference of dipolar moments of excited ions created by electron recollisions explains this behavior.

The localization dynamics of excitons in organic semiconductors influence the efficiency of charge transfer and separation in these materials. Here we apply time-resolved X-ray absorption spectroscopy to track photoinduced dynamics of a paradigmatic crystalline conjugated polymer: poly(3-hexylthiophene) (P3HT) commonly used in solar cell devices. The π→π^* transition, the first step of solar energy conversion, is pumped with a 15 fs optical pulse and the dynamics are probed by an attosecond soft X-ray pulse at the carbon K-edge. We observe X-ray spectroscopic signatures of the initially hot excitonic state, indicating that it is delocalized over multiple polymer chains. This undergoes a rapid evolution on a sub 50 fs timescale which can be directly associated with cooling and localization to form either a localized exciton or polaron pair.