Effect of cluster expansion on photoionization of iron pentacarbonyl doped inert gas clusters under gigawatt intensity laser irradiation

RATIONALE The aim of the investigation was to understand the variation in ionization dynamics of inert gas clusters upon doping with species with lower ionization energy than the inert gas constituent. It was postulated that the use of dopant species having lower ionization energy would lead to facile ionization of doped inert gas clusters, resulting in enhancement of the charge state of atomic ions compared with those obtained for pure inert gas clusters. METHODS Inert gas clusters (Arn, Krn or Xen) doped with iron pentacarbonyl were generated by supersonic expansion and subjected to gigawatt intensity laser pulses (266, 355, 532 and 1064 nm wavelengths) obtained from a nanosecond Nd:YAG laser. The ions generated upon laser‐cluster interaction were characterized using a time‐of‐flight mass spectrometer. RESULTS Upon interaction of the laser with the doped inert gas clusters, the charge states of the atomic ions were found to increase with the laser wavelength. However, the highest observed charge states were found to be lower for doped inert gas clusters than for pure inert gas clusters, at all laser wavelengths. CONCLUSIONS Wavelength‐dependent generation of multiply charged atomic ions has been explained based on the three stage model, i.e. multiphoton ionization ignited‐inverse bremsstrahlung heating, and electron ionization. This model explains enhancement in the charge state of atomic ions with increasing wavelength based on inverse bremsstrahlung heating of the inner ionized electron, which is a more efficient process at longer wavelengths. Inefficient coupling of laser energy in the case of doped inert gas clusters compared with pure inert gas clusters has been rationalized on the basis of accelerated disintegration of the cluster due to facile initial ionization of dopant molecules having low ionization energy. The results suggest that a longer laser wavelength and a slower rate of cluster expansion facilitate the efficient transfer of optical energy into cluster systems. Copyright © 2012 John Wiley & Sons, Ltd.