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Intense ultrashort laser pulse irradiation of solid targets wassystematically investigated at the first-principles level, both theoreticallyand computationally. In the method, the propagation of a pulsed light through athin film is described by a one-dimensional Maxwell's equation, and themicroscopic electronic motion at different positions in the film is describedby employing first-principles time-dependent density functional theory (TDDFT).The method uses a coarse-graining approximation to couple light propagation andelectronic motion, and is termed the multiscale Maxwell-TDDFT method. Thereflectance, transmittance, and absorbance of pulsed light incident normally onthin films of 50-200 nm thickness were calculated for materials with differentoptical properties, such as aluminum (simple metal), graphite (semi-metal),silicon (small-gap dielectric), and quartz (wide-gap dielectric). Opticalresponse transitions were explored as the light intensity shifted from thelinear regime, represented by the dielectric function for weak light, to theextremely nonlinear regime, represented by plasma reflection under intenselight conditions. Numerous mechanisms that depend on the laser pulse intensityand material type were found to contribute to these changes. These includemultiphoton absorption, saturable absorption, sign change of the effectivedielectric constant, and transition from quantum occupation to classicalBoltzmann distribution. Thus, the calculations provide a unified understandingof the interaction of intense pulsed light with solids, occurring on anextremely short time scale.

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