Interaction of intense ultrashort laser pulses with solid targets: A systematic analysis using first-principles calculations

Intense ultrashort laser pulse irradiation of solid targets was systematically investigated at the first-principles level, both theoretically and computationally. In the method, the propagation of a pulsed light through a thin film is described by a one-dimensional Maxwell's equation, and the microscopic electronic motion at different positions in the film is described by employing first-principles time-dependent density functional theory (TDDFT). The method uses a coarse-graining approximation to couple light propagation and electronic motion, and is termed the multiscale Maxwell-TDDFT method. The reflectance, transmittance, and absorbance of pulsed light incident normally on thin films of 50–200 nm thickness were calculated for materials with different optical properties, such as aluminum (simple metal), graphite (semimetal), silicon (small-gap dielectric), and quartz (wide-gap dielectric). Optical response transitions were explored as the light intensity shifted from the linear regime, represented by the dielectric function for weak light, to the extremely nonlinear regime, represented by plasma reflection under intense light conditions. Numerous mechanisms that depend on the laser pulse intensity and material type were found to contribute to these changes. These include multiphoton absorption, saturable absorption, sign change of the effective dielectric constant, and transition from quantum occupation to classical Boltzmann distribution. Thus, the calculations provide a unified understanding of the interaction of intense pulsed light with solids, occurring on an extremely short timescale.