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

Augmented collisional ionization via excited states in XUV cluster interactions