A fully analytical method for calculating Born charges and, hence, infrared intensities of periodic systems, is formulated and implemented in the CRYSTAL program, which uses a local Gaussian type basis set. Our efficient formalism combines integral gradients with first-order coupled perturbed Hartree–Fock/Kohn Sham electronic response to an electric field. It avoids numerical differentiation with respect to wave vectors, as in some Berry phase approaches, and with respect to atomic coordinates. No perturbation equations for the atomic displacements need to be solved. Several tests are carried out to verify numerical stability, consistency in one, two, and three dimensions, and applicability to large unit cells. Future extensions to piezoelectricity and Raman intensities are noted.

Ab initio analytical infrared intensities for periodic systems through a coupled perturbed Hartree-Fock/Kohn-Sham method

MASCHIO, LORENZO;ORLANDO, Roberto;
2012

Abstract

A fully analytical method for calculating Born charges and, hence, infrared intensities of periodic systems, is formulated and implemented in the CRYSTAL program, which uses a local Gaussian type basis set. Our efficient formalism combines integral gradients with first-order coupled perturbed Hartree–Fock/Kohn Sham electronic response to an electric field. It avoids numerical differentiation with respect to wave vectors, as in some Berry phase approaches, and with respect to atomic coordinates. No perturbation equations for the atomic displacements need to be solved. Several tests are carried out to verify numerical stability, consistency in one, two, and three dimensions, and applicability to large unit cells. Future extensions to piezoelectricity and Raman intensities are noted.
137
204113
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http://jcp.aip.org/resource/1/jcpsa6/v137/i20/p204113_s1
Ab initio calculations; Berry phase; GTO calculations; HF calculations; infrared spectra; piezoelectricity; Raman spectra; spectral line intensity
Lorenzo Maschio; Bernard Kirtman; Roberto Orlando; Michel Rèrat
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Utilizza questo identificativo per citare o creare un link a questo documento: http://hdl.handle.net/2318/130195
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