Quantum kinetic theory of nonlinear optical currents: Finite Fermi surface and Fermi sea contributions

Abstract

The quantum kinetic framework provides a versatile method for investigating the dynamical optical and transport currents of crystalline solids. In this paper, starting from the density-matrix equations of motion, we present a general theoretical path to obtain the nonlinear optical response in an elegant and transparent manner. We devise an extensive kinetic theory that can be applied to materials with arbitrary band structures and captures intraband and interband coherence effects, finite Fermi surfaces, and disorder effects. We present a classification of the nonlinear optical currents arising from the interference of the interband and intraband components of the density matrix with distinct symmetry and quantum geometrical origin for each contribution. In this context, we report the following four primary findings: (i) The Fermi golden rule approach is insufficient to derive the correct expression for the injection current, a shortcoming that we remedy in our theory while associating the injection current with the intraband-interband contribution to the second-order density matrix. (ii) The interband-intraband contribution yields a resonant current that survives irrespective of any symmetry constraint in addition to the well-known anomalous nonlinear current (nonresonant), which requires time-reversal symmetry. (iii) Quite generally, the nonlinear current is significantly enhanced by contributions arising from the finite Fermi surface. (iv) The finite Fermi surface and Fermi sea additionally lead to sizable novel nonlinear effects via contributions we term double resonant and higher-order pole. We investigate such effects in sum frequency and difference frequency generation. As an illustration, we compute the nonlinear response of the topological antiferromagnet CuMnAs and thin film tilted Weyl semimetals as model systems dominated by interband coherence contributions. We find that the nonlinear response of CuMnAs is responsive to the direction of the finite magnetization field and the response of Weyl semimetal to the tilt. In addition, the choice of the polarization angle of the beam is crucial to have a nonlinear current in CuMnAs, while it is not the case for Weyl semimetals.