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弛豫铁电体钛酸铋钠（Na0.5Bi0.5TiO3,NBT）具有优异的铁电性能，被广泛认为是极具应用前景的无铅铁电材料。深入阐明其在高压下的结构演化规律与相变机理，对于推动这类环境友好型铁电材料的应用至关重要。本研究结合原位高压中子衍射实验与第一性原理计算，研究了NBT在高压下的结构演化规律。高压中子衍射实验结果表明，NBT的常压相R3c相和高压相Pnma相的共存压力区间为1.1-4.6 GPa，其体积模量分别为89.3 GPa和108.6 GPa。通过分析压力诱导的微观结构演变，本研究阐明了NBT高压相与常压相在微观结构特征上的差异及对体积模量的影响，建立了高压下NBT的微观结构响应与宏观物理性能的内在联系。获得的相关结论为无铅压电材料的高压性能调控提供了重要的实验依据与参考。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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