In situ X‐ray diffraction investigation of electric‐field‐induced switching in a hybrid improper ferroelectric

Improper ferroelectric mechanisms are increasingly under investigation for their potential to expand the current catalogue of functional materials whilst promoting couplings between ferroelectricity and other technologically desirable properties such as ferromagnetism. This work presents the results of an in situ synchrotron X‐ray diffraction experiment performed on samples of Ca 2.15 Sr 0.85 Ti 2 O 7 in an effort to elucidate the mechanism of hybrid improper ferroelectric switching in this compound. By simultaneously applying an electric field and recording diffraction patterns, shifts in the intensity of superstructure peaks consistent with one of the switching mechanisms proposed by Nowadnick & Fennie [ Phys. Rev. B , (2016), 94 , 104105] are observed. While the experiment only achieves a partial response, comparison with simulated data demonstrates a preference for a one‐step switching mechanism involving an unwinding of the octahedral rotation mode in the initial stages of switching. These results represent some of the first reported experimental diffraction‐based evidence for a switching mechanism in an improper ferroelectric.