Squeezing dynamical singlets in bilayer nickelates

Abstract

We present realistic calculations within the density functional plus cluster dynamical mean-field formalism indicating that the physics of the the bilayer Ruddlesden-Popper nickelates is to a significant extent controlled by interlayer "dynamical singlets'' which are formed from the $3z^{2}-r^{2}$ orbitals singly occupied by electrons and are hybridized with itinerant planar $x^{2}-y^{2}$ orbitals. The hybridization is found to respond differently to hydrostatic pressure and to epitaxial strain, capturing the experimentally observed dichotomy between bulk single crystals and epitaxial thin films and reproducing several experimental results including angle-resolved photoemission and transport measurements.