压力诱导的s,p-d电子重分布伴随非晶Zr-Cu合金在压缩下的结构转变
Pressure-induced s,p-d electron redistribution accompanies structural transformation in amorphous Zr-Cu alloy under compression
- Warsaw University of Technology（华沙理工大学）
- Cranfield University（克兰菲尔德大学）
- The University of Bristol（布里斯托大学）
- Diamond Light Source（钻石光源）
- University of Edinburgh（爱丁堡大学）
- Ehime University（爱媛大学）
机构由 AI 辅助整理，请以论文原文为准。
AI总结：
本研究通过高压实验与模拟，揭示非晶Zr-Cu合金在压缩下发生s,p-d电子重分布，并关联其异常结构演变。
AI中文摘要：
极端压缩可以重组原子价态，在某些情况下将电荷从空间扩展轨道驱动到更紧凑的轨道。我们通过结合高达69 GPa的高压X射线吸收精细结构测量、分子动力学模拟和密度泛函理论计算，研究了非晶Zr67Cu33金属玻璃中的这一效应。Zr K边XANES光谱显示前边缘强度显著增加，且其压力依赖性发生变化，而Cu的响应明显较弱。分子动力学模拟重现了测量的EXAFS光谱，并为电子结构计算提供了可靠的输入。计算的Mulliken布居数揭示了压力诱导的Zr s和p态耗竭，伴随d态布居增加，而态密度表明压缩下p-d杂化增强。这些结果为锆中压力诱导的s,p-d电子重分布提供了实验和计算证据，并将此效应与先前报道的压缩非晶合金的异常结构演变联系起来。
英文摘要：
Extreme compression can reorganize atomic valence states, in some regimes driving charge from spatially extended orbitals into more compact ones. We investigate this effect in amorphous Zr67Cu33 metallic glass by combining high-pressure X-ray absorption fine structure measurements up to 69 GPa with molecular dynamics simulations and density functional theory calculations. The Zr K-edge XANES spectra show a pronounced increase in the pre-edge intensity and a change in its pressure dependence, whereas the Cu response is markedly weaker. Molecular-dynamics simulations reproduce the measured EXAFS spectra and provide reliable input for the electronic-structure calculations. The calculated Mulliken populations reveal pressure-induced depletion of Zr s and p-states, accompanied by an increase of the d-state population, while the density of states indicates enhanced p-d hybridization under compression. These results provide experimental and computational evidence for pressure-induced s,p-d electronic redistribution in zirconium and link this effect to the previously reported anomalous structural evolution of the compressed amorphous alloy.
