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\textit{Ab initio} second-order nonlinear optics in solids: Second-harmonic generation spectroscopy from time-dependent density-functional theory

Title\textit{Ab initio} second-order nonlinear optics in solids: Second-harmonic generation spectroscopy from time-dependent density-functional theory
Publication TypeJournal Article
Year of Publication2010
AuthorsLuppi, E., Hübener H., & Veniard V.
Abstract

We present in detail the formulation of the ab initio theory we have developed for the calculation of the macroscopic second-order susceptibility χ(2). We find a general expression for χ(2) valid for any fields, containing the ab initio relation between the microscopic and macroscopic formulation of the second-order responses. We consider the long-wavelength limit and we develop our theory in the time-dependent density-functional theory framework. This allows us to include straightforwardly many-body effects such as crystal local-field and excitonic effects. We compute the second-harmonic generation spectra for the cubic semiconductors SiC, AlAs, and GaAs and starting from the independent-particle approximation for χ(2), we include quasiparticle effects via the scissors operator, crystal local-field, and excitonic effects. In particular, we consider two different types of kernels: the adiabatic local-density approximation and the “long-range” kernel. We find good agreement with other theoretical calculations and experiments presented in literature, showing the importance of very accurate description of the many-body interactions.

JournalPhysical Review B
Volume82
Pagination235201
URLhttp://dx.doi.org/10.1103/PhysRevB.82.235201
Date Published2010/Dec//
Citation Key1192