Application to nonlinear optical properties of the RSX-QIDH double-hybrid range-separated functional

Abstract

The effective calculation of static nonlinear optical properties requires a considerably high accuracy at a reasonable computational cost, to tackle challenging organic and inorganic systems acting as precursors and/or active layers of materials in (nano-)devices. That trade-off implies to obtain very accurate electronic energies in the presence of externally applied electric fields to consequently obtain static polarizabilities ( ${\alpha }_{ij}$ ) and hyper-polarizabilities ( ${\beta }_{ijk}$ and ${\gamma }_{ijkl}$ ). Density functional theory is known to provide an excellent compromise between accuracy and computational cost, which is however largely impeded for these properties without introducing range-separation techniques. We thus explore here the ability of a modern (double-hybrid and range-separated) Range-Separated eXchange Quadratic Integrand Double-Hybrid exchange-correlation functional to compete in accuracy with more costly and/or tuned methods, thanks to its robust and parameter-free nature.

Keywords: density functional theory; double‐hybrid density functionals; nonlinear optical properties.