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We perform a frequency-resolved analysis of electron dynamics in solids toobtain microscopic insight into linear and nonlinear optical phenomena. For theanalysis, we first compute the electron dynamics under optical electric fieldsand evaluate the microscopic current density as a function of time and space.Subsequently, we perform the Fourier transformation on the microscopic currentdensity and obtain the corresponding quantity in the frequency domain. Thefrequency-resolved microscopic current density provides insight into themicroscopic electron dynamics in real-space at the frequency of linear andnonlinear optical responses. We apply frequency-resolved microscopic currentdensity analysis to light-induced electron dynamics in aluminum, silicon, anddiamond based on the first-principles electron dynamics simulation according tothe time-dependent density functional theory. Consequently, the nature ofdelocalized electrons in metals and bound electrons in semiconductors andinsulators is suitably captured by the developed scheme.

Frequency-resolved microscopic current density analysis of linear and nonlinear optical phenomena in solids