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When a nanoparticle is irradiated by an intense laser pulse, it turns into a nanoplasma, a transition that is accompanied by many interesting nonequilibrium dynamics. So far, most experiments on nanoplasmas use ion measurements, reflecting the outside dynamics in the nanoparticle. Recently, the direct observation of the ultrafast structural dynamics on the inside of the nanoparticle also became possible with the advent of x-ray free electron lasers (XFELs). Here, we report on combined measurements of structural dynamics and speeds of ions ejected from nanoplasmas produced by intense near-infrared laser irradiations, with the control of the initial plasma conditions accomplished by widely varying the laser intensity (9×1014 W/cm2 to 3×1016 W/cm2). The structural change of nanoplasmas is examined by time-resolved x-ray diffraction using an XFEL, while the kinetic energies of ejected ions are measured by an ion time-of-fight method under the same experimental conditions. We find that the timescale of crystalline disordering in nanoplasmas strongly depends on the laser intensity and scales with the inverse of the average speed of ions ejected from the nanoplasma. The observations support a recently suggested scenario for nanoplasma dynamics in the wide intensity range, in which crystalline disorder in nanoplasmas is caused by a rarefaction wave propagating at a speed comparable with the average ion speed from the surface toward the inner crystalline core. We demonstrate that the scenario is also applicable to nanoplasma dynamics in the hard x-ray regime. Our results connect the outside nanoplasma dynamics to the loss of structure inside the sample on the femtosecond timescale.
A central motivation for the development of x-ray free-electron lasers has been the prospect of time-resolved single-molecule imaging with atomic resolution. Here, we show that x-ray photoelectron diffraction—where a photoelectron emitted after x-ray absorption illuminates the molecular structure from within—can be used to image the increase of the internuclear distance during the x-ray-induced fragmentation of an O2 molecule. By measuring the molecular-frame photoelectron emission patterns for a two-photon sequential K-shell ionization in coincidence with the fragment ions, and by sorting the data as a function of the measured kinetic energy release, we can resolve the elongation of the molecular bond by approximately 1.2 a.u. within the duration of the x-ray pulse. The experiment paves the road toward time-resolved pump-probe photoelectron diffraction imaging at high-repetition-rate x-ray free-electron lasers.