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Density-functional perturbational theory for dielectric tensors in the ultrasoft pseudopotential scheme

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Umari, P Gonze, Xavier [UCL] Pasquarello, A

We introduce a density-functional perturbational scheme based on ultrasoft pseudopotentials for calculating dielectric tensors of periodic systems. We obtain a variational functional for the second-order derivative of the energy with respect to an electric field. Our scheme makes use of the correspondence between all-electron and pseudo-wave-functions introduced in the projector augmented wave method. While we here specifically focus on ultrasoft pseudopotentials, our scheme also covers the case of norm-conserving ones. In the latter case, our formulation coincides with earlier ones but highlights the implied approximations. By construction, our scheme also applies to the all-electron projector augmented wave method. We first assess the validity of our scheme by calculating polarizability tensors and Raman intensities of small molecules (H2O, CH4, NH3). We find good agreement with both experimental data and previous all-electron results. We then illustrate the potential of our scheme for treating systems of relatively large size through an application to a disordered model structure of vitreous silica.

Document type Article de périodique (Journal article) – Article de recherche
Access type Accès restreint
Publication date 2004
Language Anglais
Journal information "Physical review. B, Condensed matter and materials physics" - Vol. 69, no. 23, p. 235102:1-11 (2004)
Peer reviewed yes
Publisher American Physical Soc (College Pk)
issn 1098-0121
Publication status Publié
Affiliation UCL - FSA/MAPR - Département des sciences des matériaux et des procédés
Links
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Bibliographic reference Umari, P ; Gonze, Xavier ; Pasquarello, A. Density-functional perturbational theory for dielectric tensors in the ultrasoft pseudopotential scheme. In: Physical review. B, Condensed matter and materials physics, Vol. 69, no. 23, p. 235102:1-11 (2004)
Permanent URL http://hdl.handle.net/2078.1/40091