Abstract

Achieving effective tuning of glass structures between distinct states is intriguing for fundamental studies and applications, but has previously turned out to be challenging in practice. High-entropy metallic glasses (HEMGs), as an emerging type of metallic glasses (MGs) based on the high-entropy effect, are expected to have more disordered and frustrated chemical short-range structure compared with conventional MGs. Therefore, HEMGs may offer possibilities for structure and properties tuning in glasses. In this work, we employ pressure as a tuning parameter and monitor the atomic structural evolution of a senary HEMG, ${\mathrm{Ti}}_{16.7}{\mathrm{Zr}}_{16.7}{\mathrm{Hf}}_{16.7}{\mathrm{Cu}}_{16.7}{\mathrm{Ni}}_{16.7}{\mathrm{Be}}_{16.7}$, up to \ensuremath{\sim}40 GPa using in situ synchrotron x-ray diffraction. Analysis of its structure factor in reciprocal space and reduced pair distribution function in real space both reveal a pressure-induced structural crossover at \ensuremath{\sim}20 GPa with a dramatic change in short-range order (SRO), while no similar phenomenon is observed in a conventional MG, ${\mathrm{Cu}}_{36}{\mathrm{Zr}}_{64}$, as a control sample, suggesting the pressure-induced highly tunable SRO in HEMGs originates from the local chemical complexity, namely, the high-entropy effect. These results confirm that enhanced flexibility and tunability of atomic structures could be achieved by introducing the high-entropy effect into MGs. Therefore, configurational entropy could be another dimension for exploring MGs with highly tunable structures and properties for various potential applications.

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