Molecular Quadratic Response Properties with Inclusion of Relativity

This dissertation is about quadratic response properties as well as their application to properties in Jablonski diagrams like resonant two-photon absorption and excited state absorption. The primary focus is in optical power limiting applications, and in this perspective, molecules that contains heavy metal atoms prove superior. Thus, we’re focused on how relativity impacts these properties, and in order to evaluate this, a four-component relativistic framework is used. To correctly deal with the molecular properties of interest, both relativistic effects and electron correlation must be taken into account. Both of these properties aren’t additive, and, hence, correlation has to be integrated into the four-component framework. We present the implementation of quadratic response properties at the four-component density functional level of theory. For second-harmonic generation, we’ve, with mathematical illustrations, revealed that correlation and relativity really are not additive and that the inclusion of noncollinear magnetization is of small value. We report that both electron correlation as well as relativity strongly affect results for second-harmonic generation. For instance, relativity alone lowers µß-response signal by 62% and 75% for meta- and ortho-bromobenzene, respectively, and improves the same response by 17% and 21% for meta- and ortho-iodobenzene, respectively…

Contents: Molecular Quadratic Response Properties with Inclusion of Relativity

1 Introduction
1.1 Optical Power Limiting
1.2 Passive Protection and Jablonski Diagrams
1.3 Active Protection and Spin-transitions
2 Molecular Electronic-structure Theory
2.1 Self-consistent Field Theory
2.1.1 Wave Function Methods
2.1.2 Density Functional Theory
2.1.3 Relativistic Considerations
2.2 Basis Sets
2.2.1 Effective Core Potentials
2.3 Response Theory
2.3.1 Electric Field Induced Response Functions
3 Clamping Levels in Optical Power Limiting…

Source: Linköping University

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