First-principles theory of spatial dispersion: Dynamical quadrupoles and flexoelectricity

Abstract

Density-functional perturbation theory (DFPT) is nowadays the method of choice for the accurate computation of linear and non-linear response properties of materials from first principles. A notable advantage of DFPT over alternative approaches is the possibility of treating incommensurate lattice distortions with an arbitrary wavevector, $\mathbf{q}$, at essentially the same computational cost as the lattice-periodic case. Here we show that $\mathbf{q}$ can be formally treated as a perturbation parameter, and used in conjunction with established results of perturbation theory (e.g. the "2n+1" theorem) to perform a long-wave expansion of an arbitrary response function in powers of the wavevector components. This provides a powerful, general framework to accessing a wide range of spatial dispersion effects that were formerly difficult to calculate by means of first-principles electronic-structure methods. In particular, the physical response to the spatial gradient of any external field can now be calculated at negligible cost, by using the response functions to $uniform$ perturbations (electric, magnetic or strain fields) as the only input. We demonstrate our method by calculating the flexoelectric and dynamical quadrupole tensors of selected crystalline insulators and model systems.

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