Spin-Opposite-Scaled Range-Separated Exchange Double-Hybrid Models (SOS-RSX-DHs): Marriage Between DH and RSX/SOS-RSX Is Not Always a Happy Match.

The range-separated version of double-hybrid density functional theory (DH-DFT) with a remarkable efficiency for both ground-state and excited-state characteristics has recently come into spotlight. In this work, based on theoretical arguments, several variants of spin-opposite-scaled range-separated exchange double-hybrid models (SOS-RSX-DHs) have been proposed and validated. More specifically, we first extend the RSX-DHs to design some other related models. Next, the SOS version of the resulting approximations is constructed and thoroughly evaluated using standard benchmark compilations of various properties. It is shown that although there are properties for which the RSX-DH and SOS-RSX-DH frameworks are rival, there are still some problems particularly prone to the self-interaction error issues where our proposed models seem to be beneficial. Furthermore, some of the presented models devoid of any additional corrections can also surpass the recently proposed approximations from different rungs of "Jacob's Ladder". Nonetheless, perusing the results of different methods and detailed comparisons with the predecessors discloses that all things may not necessarily be well with the RSX and SOS-RSX schemes, where the parent DHs as well as their SOS counterparts can still come into play.