Spin and diamagnetism in linear and nonlinear optics

Abstract

We present a local-field theory for spin and diamagnetism in linear and nonlinear optics. We examine all the processes contained in the Pauli Hamiltonian and its corresponding microscopic current density, including the terms depending on the electron spin. The resulting general real-space conductivities are presented and discussed. To quantify the implications of including the spin, we study the linear and nonlinear optical properties of free-electron metals, represented by the screened homogeneous electron gas. The real-space formalism is transformed into Fourier space, and the symmetries of the linear and nonlinear optical conductivities in a homogeneous electron gas are discussed. Numerical results are presented for the homogeneous electron gas, in which we treat {omega} and q as independent variables, thereby opening the theory to near-field optics and the study of evanescent waves. We show that in regions of the {omega}-q spectrum, the presence of diamagnetism and spin dynamics significantly alters the response in comparison to considering only the paramagnetic response. Additionally, we discuss the effects of screening, and we finish our treatment by a discussion of how to connect the present theory to existing methods in ab initio solid-state physics.