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The existence of a 'crossover region' in glass-forming liquids has long beenconsidered as a general phenomenon that is as important as the glasstransition. One potential origin for the crossover behavior is aliquid-to-liquid phase transition (LLPT). Although a LLPT is thought to existin all forms of liquids, structural evidence for this, particularly insupercooled liquids, is scarce, elusive, and in many cases controversial. A keychallenge to the search for a LLPT in a supercooled liquid is the interferenceof crystallization during cooling. Crystallization induces major structuralchanges, which can overwhelm and therefore mask the more subtle changesassociated with a LLPT. Here, we report the results of an in-situ containerlesssynchrotron study of a metallic-glass-forming liquid (Zr57Nb5Al10Cu15.4Ni12.6)that show distinct changes in the liquid structure at ~1000 K, a temperaturewell below the melting temperature of the liquid and 150 K above thecrystallization temperature. The structural transition is characterized bygrowing short- and extended-range order below the transition temperature, andis accompanied by a concurrent change in density. These data provide strongevidence for a LLPT in the supercooled metallic liquid, particularly in thelight of a recent computer simulation study. That a LLPT is found in a metallicliquid supports the increasingly widely held view that a LLPT may be a commonfeature of a variety of liquids.

Liquid-to-liquid phase transition underlying the structural crossover in a supercooled metallic liquid