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We adapted a recently proposed framework to characterize the optical responseof interacting electrons in solids in order to expedite its computation withoutcompromise in accuracy at the microscopic level. Our formulation is based onreliable parameterizations of Hamiltonians and Coulomb interactions, whichallows economy and flexibility in obtaining response functions. It is suited tocomputing the optical response to fields of arbitrary temporal shape andstrength, to arbitrary order in the field, and natively accounts for excitoniceffects. We demonstrate the approach by computing the frequency-dependentsusceptibilities of MoS2 and hexagonal BN monolayers up to the third-harmonic.Grounded on a generic non-equilibrium many-body perturbation theory, thisframework allows extensions to handle generic interaction models or to describeelectronic processes taking place at ultrafast time scales.

Expeditious computation of nonlinear optical properties of arbitrary order with native electronic interactions in the time domain