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Relaxor ferroelectric sodium bismuth titanate (Na0.5Bi0.5TiO3, NBT) exhibits outstanding ferroelectric characteristics and is widely recognized as a highly promising lead-free ferroelectric material. In order to further promote the application of such environmentally friendly ferroelectric materials, it is crucial to gain a comprehensive understanding of their structural evolution and phase transition mechanisms under high pressure. This study investigates the structural evolution of NBT under hydrostatic pressure up to 6.8 GPa by integrating in situ high-pressure neutron diffraction experiments with first-principles calculations. Based on high-pressure neutron diffraction experiments conducted at the China Mianyang Research Reactor (CMRR), Rietveld refinement analysis determined the phase transition from the ambient-pressure R3c phase to the high-pressure Pnma phase in NBT, with a coexistence pressure range of 1.1–4.6 GPa. The bulk modulus of the high-pressure phase Pnma was experimentally determined for the first time, with a value of 108.6 GPa. First-principles calculations further corroborated the thermodynamic tendency for the pressure-induced phase transition from R3c to Pnma and yielded a bulk modulus in close agreement with the experimental value. By correlating with the experimentally obtained trends of the internal [TiO6] oxygen octahedral structural changes under high pressure in both phases, this study demonstrates that the difference in their macroscopic compressibility originates from the significantly higher pressure sensitivity of the oxygen octahedral distortion degree in the R3c phase compared to the Pnma phase. This relatively softer internal microstructure results in a lower bulk modulus than that of the Pnma phase. By providing a detailed analysis of the pressure-induced phase transition and microstructural evolution, this study clarifies the relationship between the microscopic structural features of the high-pressure and ambient-pressure phases of NBT and their influence on macroscopic mechanical properties, thereby establishing a fundamental connection between microscopic structural responses and bulk physical behavior under high-pressure conditions. These findings provide crucial experimental data and theoretical support for further enhancing the high-pressure performance and applications of lead-free ferroelectric materials.
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Keywords:
- Sodium Bismuth titanate /
- High-Pressure Neutron Diffraction /
- First-Principles Calculation /
- Phase Transition
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