The effect of pressure on the mechanical and physical properties of metallic glasses (MGs) has been widely reported. In experiments, it remains challenging to mechanically loading the materials under extreme hydrostatic pressures and carrying out the corresponding measurements. Here, we investigate the pressure dependence of shear response of a typical brittle FeP MG by using molecular dynamics (MD) simulations. We show that the plastic deformation of this MG loaded at a pressure below 10 GPa is highly localized in the form of a dominant shear band. The plastic flow stress during shear banding is measured to increase with the applied pressure, leading to a pressure-induced strengthening behavior at pressures in the range of 0–10 GPa. As the pressure is increased to a critical pressure of approximately 15 GPa, there occurs a transition in the deformation mechanism from localized shear banding to a delocalized shear deformation mechanism governed by the uniform activation of individual shearing events in the material. At this critical pressure, both the yield strength and the average flow stress are maximized. Further increasing the pressure lowers the strength of the material. The pressure effect on the evolution of different types of atomic clusters is analyzed, revealing that the pressure-sensitivity of atomic clusters in MGs is related to their structural symmetry. Under high hydrostatic pressures, low-symmetry clusters become sluggish due to their larger pressure sensitivity. In such circumstances, high-symmetry clusters with lower pressure sensitivity are relatively more active during shear deformation and evenly distributed in the whole sample, leading to the uniform plastic deformation at high pressures. Our findings calls for further experimental investigations of the effect of pressure on mechanical properties and deformation mechanisms of MGs.

压力对金属玻璃（MGs）的机械和物理性能的影响已被广泛报道。在实验中，在极高的静水压力下机械加载材料并执行相应的测量仍然具有挑战性。在这里，我们通过使用分子动力学（MD）模拟研究典型的脆性FeP MG剪切响应的压力依赖性。我们表明，在低于10 GPa的压力下加载的MG的塑性变形以局部剪切带的形式高度局限。测量剪切带期间的塑性流动应力会随着所施加的压力而增加，从而导致在0-10 GPa的压力下压力引起的强化行为。随着压力增加到大约15 GPa的临界压力，变形机理从局部剪切带到局部剪切剪切变形机制发生了转变，这取决于材料中各个剪切事件的均匀激活。在此临界压力下，屈服强度和平均流动应力均最大化。进一步增加压力会降低材料的强度。分析了压力对不同类型原子团簇演化的影响，揭示了MG中原子团簇的压力敏感性与它们的结构对称性有关。在高静水压力下，低对称性簇由于其较大的压力敏感性而变得缓慢。在这种情况下，压力敏感性较低的高对称簇在剪切变形期间相对较活跃，并均匀地分布在整个样本中，导致在高压下均匀的塑性变形。我们的发现要求对压力对MG的机械性能和变形机理的影响进行进一步的实验研究。