Nucleation and growth of polar clusters with in-phase tilts into a long-range ferroelectric matrix in a sodium niobate based complex relaxor

Kumar, Harsh; Ghose, Sanjit K.; Erasmus, Rudolph; Tripathi, Saurabh

doi:10.1103/szgf-l5rt

Title: Nucleation and growth of polar clusters with in-phase tilts into a long-range ferroelectric matrix in a sodium niobate based complex relaxor

Journal Article · Mon Jun 23 00:00:00 UTC 2025 · Physical Review B

DOI: https://doi.org/10.1103/szgf-l5rt · OSTI ID:2587805

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Indian Inst. of Technology (BHU), Varanasi (India)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Univ. of the Witwatersrand, Johannesburg (South Africa)

In this study, we have investigated the temperature dependence of atomic ordering at multiple length scales in a lead-free sodium niobate-based relaxor, i.e., 0.75 NaNbO₃-0.25 Ba_0.9⁢Ca_0.1⁢TiO₃ (NN-25BCT) via synchrotron x-ray diffraction, Raman spectroscopy, and pair distribution function analysis. High-resolution synchrotron x-ray powder diffraction (SXRD) measurements reveal a ferroelectric phase transition in the relaxor ferroelectric NN-25BCT below the Vogel-Fulcher freezing temperature (𝑇_VF ≈ 270 K). In addition, SXRD analysis demonstrates the competition between in-phase octahedral tilting and ferroelectric order at the long-range scale using mode crystallography. On the other hand, Raman spectroscopic analysis provides evidence of polar ordering for 𝑇 > 𝑇_VF (with tetragonal symmetry) persisting up to the Burns temperature (𝑇_B). Furthermore, pair distribution function (PDF) analysis reveals the presence of a polar antiferrodistortive tetragonal phase with 𝑃⁢4⁢𝑏𝑚 space group at short ranges throughout the studied temperatures (i.e., 110 K ≤ 𝑇 ≤500 K), irrespective of nonpolar long-range ordering above 𝑇_VF. Therefore, our measurements provide direct evidence for the presence of polar ordering at short ranges and their gradual transformation into long-range polar ordering using an integrated multiscale structural analysis. In conclusion, as a result of a transition from relaxor to a ferroelectric phase in the vicinity of room temperature, NN-25BCT can be exploited for applications in pyroelectric detectors, electrocaloric devices, and multilayered ceramic capacitors.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: Defence Research and Development Organisation; Science and Engineering Research Board (DST-SERB), Government of India; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012704

OSTI ID:: 2587805

Report Number(s):: BNL--228878-2025-JAAM

Journal Information:: Physical Review B, Journal Name: Physical Review B Journal Issue: 22 Vol. 111; ISSN 2469-9969; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Nucleation and growth of polar clusters with in-phase tilts into a long-range ferroelectric matrix in a sodium niobate based complex relaxor

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