Evidence of the Monopolar‐Dipolar Crossover Regime: A Multiscale Study of Ferroelastic Domains by In Situ Microscopy Techniques

Abstract The elastic interaction between kinks (and antikinks) within domain walls plays a pivotal role in shaping the domain structure, and their dynamics. In bulk materials, kinks interact as elastic monopoles, dependent on the distance between walls (d⁻¹) and typically characterized by a rigid and straight domain configuration. In this work the evolution of the domain structure is investigated, as the sample size decreases, by the means of in situ heating microscopy techniques on free‐standing samples. As the sample size decreases, a significant transformation is observed: domain walls exhibit pronounced curvature, accompanied by an increase in both domain wall and junction density. This transformation is attributed to the pronounced influence of kinks, inducing sample warping, where “dipole–dipole” interactions are dominant (d⁻²). Moreover, a critical thickness range that delineates a crossover between the monopolar and dipolar regimens is experimentally identified and corroborated by atomic simulations. These findings are relevant for in situ TEM studies and for the development of novel devices based on free‐standing ferroic thin films and nanomaterials.