Origins of Electromagnetic Radiation from Spintronic Terahertz Emitters: A Time-Dependent Density Functional Theory plus Jefimenko Equations Approach

Microscopic origins of charge currents and electromagnetic (EM) radiation generated by them in spintronic THz emitters-such as, femtosecond laser pulse-driven single magnetic layer or its heterostructures with a nonmagnetic layer hosting strong spin-orbit coupling (SOC)-remain poorly understood despite nearly three decades since the discovery of ultrafast demagnetization. We introduce a first-principles method to compute these quantities, where the dynamics of charge and current densities is obtained from real-time time-dependent density functional theory, which are then fed into the Jefimenko equations for properly retarded electric and magnetic field solutions of the Maxwell equations. By Fourier transforming different time-dependent terms in the Jefimenko equations, we unravel that in the 0.1-30 THz range the electric field of far-field EM radiation by the Ni layer, chosen as an example, is dominated by charge current pumped by demagnetization, while often invoked magnetic dipole radiation from the time-dependent magnetization of a single magnetic layer is a negligible effect. Such an effect of charge current pumping by a time-dependent quantum system, whose magnetization is shrinking while its vector does not rotate, does not require any spin-to-charge conversion via SOC effects. In the Ni/Pt bilayer, EM radiation remains dominated by the charge current within the Ni layer, whose magnitude is larger than in the case of a single Ni layer due to faster demagnetization, while often invoked spin-to-charge conversion within the Pt layer provides an additional but smaller contribution. By using the Poynting vector and its flux, we also quantify the efficiency of conversion of light into emitted EM radiation, and its angular distribution.