Open Access

Nikita Medvedev, Harald O. Jeschke, Beata Ziaja

• Part of Focus on High Energy Density Physics. In this paper, we present a novel theoretical approach, which allows the study of nonequilibrium dynamics of both electrons and atoms/ions within free-electron laser excited semiconductors at femtosecond time scales. The approach consists of the Monte-Carlo method treating photoabsorption, high-energy-electron and core-hole kinetics and relaxation processes. Low-energy electrons localized within the valence and conduction bands of the target are treated with a temperature equation, including source terms, defined by the exchange of energy and particles with high-energy electrons and atoms. We follow the atomic motion with the molecular dynamics method on the changing potential energy surface. The changes of the potential energy surface and of the electron band structure are calculated at each time step with the help of the tight-binding method. Such a combination of methods enables investigation of nonequilibrium structural changes within materials under extreme ultraviolet (XUV) femtosecond irradiation. Our analysis performed for diamond irradiated with an XUV femtosecond laser pulse predicts for the first time in this wavelength regime the nonthermal phase transition from diamond to graphite. Similar to the case of visible light irradiation, this transition takes place within a few tens of femtoseconds and is caused by changes of the interatomic potential induced by ultrafast electronic excitations. It thus occurs well before the heating stimulated by electron–phonon coupling starts to play a role. This allows us to conclude that this transition is nonthermal and represents a general mechanism of the response of solids to ultrafast electron excitations.