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Lattice defects such as oxygen vacancies, interstitials, and their complexes are present in crystalline oxide materials. In particular, anti‐Frenkel defects, which refer to charge‐neutral anion vacancy‐interstitial pairs, are strongly coupled with ferroelectric and dielectric properties as electric dipoles. However, in order to observe their macroscopic manifestation, delicate defect controls are required to the extent that electronic and ionic charges are almost completely suppressed. Here, the thermal cycle dependence of dielectric and piezoelectric properties is scrutinized in the strain‐driven morphotropic phase boundaries of multiferroic La‐substituted BiFeO3 thin films. Electrochemical impedance spectroscopy provides the Warburg feature that is considered evidence of the ionic origin. The observations are discussed based on anti‐Frenkel defects that are created or annihilated reversibly by thermal cycles through high‐temperature structural phase transition temperature or magnetic Néel temperature. The defect dipoles are spontaneously aligned by the flexoelectric effect in the phase boundaries inducing a metastable interfacial ferroelectric phase. The findings offer useful insight into defect dipoles. [ABSTRACT FROM AUTHOR]

Layered semimetals such as monoclinic MoTe2 and WTe2 demonstrate superconducting, topological insulating, and Weyl semimetallic states based on their unique electronic band topology. While doping concentration, lattice constants, and spin–orbit coupling can largely modulate the quantum states of the semimetals, a puzzling issue is that their functional carrier density and magnetoresistance for practical applications critically vary by temperature, which cannot be explained by the conventional phonon effect or a structural phase transition. Here, a native doping‐mediated thermomechanical manipulation of electric transport in semimetallic MoTe2 is reported, where effective transport is controlled by temperature in an equivalent manner to electric gating. Combining X‐ray diffraction, scanning tunneling microscopy, transport measurements, and first‐principles calculations, a Fermi level shift and subsequent changes in electronic structures are revealed as the origins of the practical transport changes in MoTe2. Moreover, the initial doping state of the MoTe2, determined by the Te vacancy density in two different growth methods, reciprocally affects the thermomechanical lattice and band structure changes, which is promising for novel electronic applications such as magnetic sensors and memory devices with layered semimetals. [ABSTRACT FROM AUTHOR]