4.8 Article

Designing Monoclinic Heterophase Coexistence for the Enhanced Piezoelectric Performance in Ternary Lead-Based Relaxor Ferroelectrics

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 14, Issue 8, Pages 10535-10545

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c22983

Keywords

relaxor ferroelectrics; nanostructure; nanodomain; phase coexistence; giant piezoelectricity

Funding

  1. National Key Research and Development Program of China [2019YFB2203400]
  2. National Natural Science Foundation of China [61974043, 62090013, 12104156, 61974044, 91833303]
  3. Projects of Science and Technology Commission of Shanghai Municipality [21JC1402100, 19511120100]
  4. China Postdoctoral Science Foundation [2020TQ0099, 2020M681222]
  5. Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning

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The study explores the development of next-generation electromechanical devices using ternary relaxor-PbTiO3 based ferroelectric crystals. Researchers have designed a monoclinic heterophase in a single crystal with optimized composition, which exhibits ultrahigh piezoelectric coefficient. Through high-resolution spectroscopic-microscopic technique, they observed two different heterophase mixtures responsible for different functionalities and correlated them with the ferroelectric-dominated and relaxor-ferroelectric-dominated nanodomain structure.
Enhanced piezoelectric, dielectric properties and thermal stability in ternary relaxor-PbTiO3 based ferroelectric crystals are expected to develop the next-generation of electromechanical devices. However, due to their increased disorder compared to other ferroelectrics, designing a controllable phase boundary structure and engineered domain remains a challenging task. Here, we construct a monoclinic heterophase coexisting in a ternary Pb(In1/2Nb1/2)O-3-Pb(Mg1/3Nb2/3)O-3-PbTiO3 single crystal with optimized composition and an ultrahigh piezoelectric coefficient of 1400 pC N-1, to quantify the correlation between spontaneous nanopolarity and phase heterogeneity, in an attempt to understand the origin of the exceptional functionalities. By designing an in situ high-resolution spectroscopic-microscopic technique, we have observed M-a and M-c heterophase mixtures spatially separated by the monoclinic heterophase boundary (MHB), which are responsible for the ferroelectric-dominated and relaxor-ferroelectric-dominated nanodomain structure, respectively. Internal energy mapping from optical soft mode dynamics reveals the inhomogeneous polarization and local symmetry on both sides of the MHB. Various molecular polarizabilities and localized octahedral distortions correlate directly with monoclinic regions and electromechanical contribution. This work clarifies the heterogeneity between structure, energy, and polar order and provides a new design freedom for advanced relaxor ferroelectrics.

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