Contributor info: Prof. Ivo Souza

Óscar Pozo Ocaña, Ivo Souza

SciPost Phys. 14, 118 (2023) · published 17 May 2023 | Toggle abstract · pdf

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 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 interband 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 wavevector of light contains band-dispersion terms that have no counterpart in molecular theories. The full response is broken down into magnetoelectric and quadrupolar parts, which can be isolated in the static limit where electric and magnetic fields become decoupled. 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.

Stepan S. Tsirkin, Ivo Souza

SciPost Phys. Core 5, 039 (2022) · published 8 August 2022 | Toggle abstract · pdf

The symmetric and antisymmetric parts of the linear conductivity describe the dissipative (Ohmic) and nondissipative (Hall) parts of the current. The Hall current is always transverse to the applied electric field regardless of its orientation; the Ohmic current is purely longitudinal in cubic crystals, but in lower-symmetry crystals it has a transverse component whenever the field is not aligned with a principal axis. In this work, we extend that analysis beyond the linear regime. We consider all possible ways of partitioning the current at any order in the electric field without taking symmetry into account, and find that the Hall vs Ohmic decomposition is the only one that satisfies certain basic requirements. A general prescription is given for achieving that decomposition, and the case of the quadratic conductivity is analyzed in detail. By performing a symmetry analysis we find that in five of the 122 magnetic point groups the quadratic dc conductivity is purely Ohmic and even under time reversal, a type of response that is entirely disorder mediated.

Julen Ibañez-Azpiroz, Fernando de Juan, Ivo Souza

SciPost Phys. 12, 070 (2022) · published 22 February 2022 | Toggle abstract · pdf

We study the role of hopping matrix elements of the position operator $\mathbf{\hat{r}}$ in tight-binding calculations of linear and nonlinear optical properties of solids. Our analysis relies on a Wannier-interpolation scheme based on ab initio calculations, which automatically includes matrix elements of $\mathbf{\hat{r}}$ between different Wannier orbitals. A common approximation, both in empirical tight-binding and in Wannier-interpolation calculations, is to discard those matrix elements, in which case the optical response only depends on the on-site energies, Hamiltonian hoppings, and orbital centers. We find that interatomic $\mathbf{\hat{r}}$-hopping terms make a sizeable contribution to the shift photocurrent in monolayer BC$_2$N, a covalent acentric crystal. If a minimal basis of $p_z$ orbitals on the carbon atoms is used to model the band-edge response, even the dielectric function becomes strongly dependent on those terms.