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Hybrid improper ferroelectricity (HIF) denotes a new class of polarinstability by the mixture of two octahedral-distortion modes and can featurethe coexistence of abundant head-to-head and tail-to-tail polar domains, ofwhich the domain walls tend to be charged due to the respective screeningcharges with an opposite sign. However, no such coexisting carriers areavailable in the materials. Using group-theoretical, microscopic, andspectroscopic analyses, we established the existence of hidden antipolar orderparameter in model HIF (Ca,Sr)3Ti2O7 by the condensation of a weak, previouslyunnoticed antipolar lattice instability, turning the order-parameter spaces tobe multicomponent with the distinct polar-antipolar intertwining andaccompanied formation of Neel-type twin-like antipolar domain walls (few nm)between the head-to-head and tail-to-tail domains. The finite-width Neel wallsand correlated domain topology inherently lift the polar divergences betweenthe domains, casting an emergent exemplification of charged domain-wallscreening by an antipolar ingredient. Comparisons to topological defects inimproper-ferroelectrics hexagonal manganites were discussed.

Hidden Antipolar Order Parameter and Entangled Neel-Type Charged Domain Walls in Hybrid Improper Ferroelectrics