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arXiv · 2302.05635

First-Principles Calculation of the Optical Rotatory Power of Periodic Systems: Modern Theory with Modern Functionals

Jacques K. Desmarais·Bernard Kirtman·Michel Rérat
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Abstract

An analysis of orbital magnetization in band insulators is provided. It is shown that a previously proposed electronic orbital angular-momentum operator generalizes the ``modern theory of orbital magnetization'' to include non-local Hamiltonians. Expressions for magnetic transition dipole moments needed for the calculation of optical rotation (OR) and other properties are developed. A variety of issues that arise in this context are critically analyzed. These issues include periodicity of the operators, previously proposed band dispersion terms as well as, if and where needed, evaluation of reciprocal space derivatives of orbital coefficients. Our treatment is used to determine the optical rotatory power of band insulators employing a formulation that accounts for electric dipole - electric quadrupole (DQ), as well as electric dipole-magnetic dipole, contributions. An implementation in the public \textsc{Crystal} program is validated against a model finite system and applied to the $\alpha$-quartz mineral through linear-response time-dependent density functional theory with a hybrid functional. The latter calculations confirmed the importance of DQ terms. Agreement against experiment was only possible with i) use of a high quality basis set, ii) inclusion of a fraction of non-local Fock exchange, and iii) account of orbital-relaxation terms in the calculation of response functions.

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Jacques K. Desmarais, Bernard Kirtman, Michel Rérat. 2023-02-11. First-Principles Calculation of the Optical Rotatory Power of Periodic Systems: Modern Theory with Modern Functionals. https://doi.org/10.1103/physrevb.107.224430

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