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Diagrammatic approach to nonlinear optical response with application to Weyl semimetals

DOI:10.1103/PhysRevB.99.045121 期刊:Physical Review B 出版年份:2019 更新时间:2025-09-23 15:23:52
摘要: Nonlinear optical responses are a crucial probe of physical systems including periodic solids. In the absence of electron-electron interactions, they are calculable with standard perturbation theory starting from the band structure of Bloch electrons, but the resulting formulas are often large and unwieldy, involving many energy denominators from intermediate states. This work gives a Feynman diagram approach to calculating nonlinear responses. This diagrammatic method is a systematic way to perform perturbation theory, which often offers shorter derivations and also provides a natural interpretation of nonlinear responses in terms of physical processes. Applying this method to second-order responses concisely reproduces formulas for the second-order-harmonic shift current. We then apply this method to third-order responses and derive formulas for third-order-harmonic generation and self-focusing of light, which can be directly applied to tight-binding models. Third-order responses in the semiclassical regime include a Berry curvature quadrupole term, whose importance is discussed including symmetry considerations and when the Berry curvature quadrupole becomes the leading contribution. The method is applied to compute third-order optical responses for a model Weyl semimetal, where we find a new topological contribution that diverges in a clean material, as well as resonances with a peculiar linear character.
作者: Daniel E. Parker,Takahiro Morimoto,Joseph Orenstein,Joel E. Moore
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To develop a Feynman diagram approach for calculating nonlinear optical responses in solids, providing a systematic and interpretable method for perturbation theory, and to apply this method to second- and third-order responses, including in Weyl semimetals.

The Feynman diagram approach provides a concise and systematic way to compute nonlinear optical responses, reproducing known results for second-order effects and enabling new insights into third-order responses. In Weyl semimetals, third-order responses show a topological divergence due to Berry curvature quadrupole and peculiar linear resonances. The method simplifies perturbation theory calculations and offers physical interpretations in terms of diagrammatic processes.

The method assumes non-interacting electrons and does not account for electron-electron interactions, which may limit applicability to strongly correlated systems. It relies on the velocity gauge, which can have spurious divergences at low frequencies that require sum rules to handle. The approach is primarily suited for analytical and tight-binding models; for quantitative predictions, density functional theory or other advanced methods may be needed. Dynamical effects like scattering and relaxation are incorporated phenomenologically but not fully from first principles.

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