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Register a new userIgnition of a helium nanoplasma by x-ray multiple ionization of a heavy rare-gas core
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The dynamics of an x-ray-ionized two-component core-shell nanosystem is probed using doped helium (He) nanodroplets. First, a soft x-ray pump pulse selectively inner-shell ionizes the core cluster formed of heavier rare-gas atoms, causing electron migration from the He shell to the highly charged core. This ignites a He nanoplasma which is then driven by an intense near-infrared probe pulse. The ultrafast charge redistribution, evidenced by the rise of He$^+$ and He$^{2+}$ ion yields from the nanoplasma within $<70$ fs, leads to strong damping of the core cluster expansion. Thus, He droplets act as efficient tampers that reduce the radiation damage of embedded nanostructures, a property that could be exploited for improving coherent diffraction images.
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We have recorded the coherent diffraction images of individual xenon clusters with intense extreme ultraviolet pulses to elucidate the influence of light-induced electronic changes on the diffraction pattern. Using the FLASH free-electron laser we tuned the wavelength to specific xenon atomic and ionic resonances. The data show the emergence of a transient core-shell structure within the otherwise homogeneous sample. Simulations indicate that ionization and nanoplasma formation result in a cluster shell with strongly altered refraction. The presented resonant scattering approach enables imaging of ultrafast electron dynamics on their natural time scale.
Helium (He) nanodroplets irradiated by intense near-infrared laser pulses form a nanoplasma by avalanche-like electron impact ionizations even at lower laser intensities where He is not directly field ionized, provided that the droplets contain a few dopant atoms which provide seed electrons for the electron impact ionization avalanche. In this theoretical paper on calcium and xenon doped He droplets we elucidate the mechanism which induces ionization avalanches, termed ignition. We find that the partial loss of seed electrons from the activated droplets starkly assists ignition, as the Coulomb barrier for ionization of helium is lowered by the electric field of the dopant cations, and this deshielding of the cation charges enhances their electric field. In addition, the dopant ions assist the acceleration of the seed electrons (slingshot effect) by the laser field, supporting electron impact ionizations of He and also causing electron loss by catapulting electrons away. The dopants ability to lower the Coulomb barriers at He as well as the slingshot effect decrease with the spatial expansion of the dopant, causing a dependence of the dopants ignition capability on the dopant mass. Here, we develop criteria (impact count functions) to assess the ignition capability of dopants, based on (i) the spatial overlap of the seed electron cloud with the He atoms and (ii) the overlap of their kinetic energy distribution with the distribution of Coulomb barrier heights at He. The relatively long time delays between the instants of dopant ionization and ignition (incubation times) for calcium doped droplets are determined to a large extent by the time it takes to deshield the dopant ions.
Helium nanodroplets irradiated by intense near-infrared laser pulses ignite and form highly ionized nanoplasmas even at laser intensities where helium is not directly ionized by the optical field, provided the droplets contain a few dopant atoms. We present a combined theoretical and experimental study of the He nanoplasma ignition dynamics for various dopant species. We find that the efficiency of dopants to ignite a nanoplasma in helium droplets strongly varies and mostly depends on (i) the pick-up process, (ii) the number of free electrons each dopant donates upon ionization, and remarkably, (iii) by the hitherto unexplored effect of the dopant location in or on the droplet.
Clusters and nanodroplets hold the promise of enhancing high-order nonlinear optical effects due to their high local density. However, only moderate enhancement has been demonstrated to date. Here, we report the observation of energetic electrons generated by above-threshold ionization (ATI) of helium (He) nanodroplets which are resonantly excited by ultrashort extreme ultraviolet (XUV) free-electron laser pulses and subsequently ionized by near-infrared (NIR) or near-ultraviolet (UV) pulses. The electron emission due to high-order ATI is enhanced by several orders of magnitude compared to He atoms. The crucial dependence of the ATI intensities with the number of excitations in the droplets suggests a local collective enhancement effect.
We demonstrate ultrafast resonant energy absorption of rare-gas doped He nanodroplets from intense few-cycle (~10 fs) laser pulses. We find that less than 10 dopant atoms ignite the droplet to generate a non-spherical electronic nanoplasma resulting ultimately in complete ionization and disintegration of all atoms, although the pristine He droplet is transparent for the laser intensities applied. Our calculations at those intensities reveal that the minimal pulse length required for ignition is about 9 fs.
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