  The impact of atomic excited states is investigated via a detailed model of
laser-cluster interactions, which is applied to rare gas clusters in intense
femtosecond pulses in the extreme ultraviolet (XUV). This demonstrates the
potential for a two-step ionization process in laser-cluster interactions, with
the resulting intermediate excited states allowing for the creation of high
charge states and the rapid dissemination of laser pulse energy. The
consequences of this excitation mechanism are demonstrated through simulations
of recent experiments in argon clusters interacting with XUV radiation, in
which this two-step process is shown to play a primary role; this is consistent
with our hypothesis that XUV-cluster interactions provide a unique window into
the role of excited atomic states due to the relative lack of photoionization
and laser field-driven phenomena. Our analysis suggests that atomic excited
states may play an important role in interactions of intense radiation with
materials in a variety of wavelength regimes, including potential implications
for proposed studies of single molecule imaging with intense X-rays.
