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We have developed a novel multiscale computational scheme to describe coupleddynamics of light electromagnetic field with electrons and atoms in crystallinesolids, where first-principles molecular dynamics based on time-dependentdensity functional theory is used to describe the microscopic dynamics. Themethod is applicable to wide phenomena in nonlinear and ultrafast optics. Toshow usefulness of the method, we apply it to a pump-probe measurement ofcoherent phonon in diamond where a Raman amplification takes place during thepropagation of the probe pulse.

Time-dependent density functional theory for a unified description of ultrafast dynamics: pulsed light, electrons, and atoms in crystalline solids