SKM 2023 – scientific programme

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CPP: Fachverband Chemische Physik und Polymerphysik

CPP 23: Optical Properties (joint session HL/CPP)

CPP 23.6: Talk

Tuesday, March 28, 2023, 11:00–11:15, POT 112

Multipole theory of optical spatial dispersion in crystals — •Óscar Pozo — Centro de Física de Materiales, Universidad del País Vasco, 20018 San Sebastián, Spain

Natural optical activity is the paradigmatic example of an effect originating in the weak spatial inhomogeneity of the electromagnetic field on the atomic scale. In molecules, such effects are well described by the multipole theory of electromagnetism, where the coupling to light is treated semiclassically beyond the electric-dipole approximation. That theory has two shortcomings: it is limited to bounded systems, and its building blocks - the multipole transition moments - are origin dependent. In this work, we recast the multipole theory in a translationally-invariant form that remains valid for periodic crystals. Working in the independent-particle approximation, we introduce 'intrinsic' multipole transition moments that are origin independent and transform covariantly under gauge transformations of the Bloch eigenstates. Electric-dipole transitions are given by the interbank Berry connection, while magnetic-dipole and electric-quadrupole transitions are described by matrix generalizations of the intrinsic magnetic moment and quantum metric. In addition to multipole-like terms, the response of crystals at first order in the wave vector of light contains band-dispersion terms that have no counterpart in molecular theories. The rotatory-strength sum rule for crystals is found to be equivalent to the topological constraint for a vanishing chiral magnetic effect in equilibrium, and the formalism is validated by numerical tight-binding calculations.