We report on the solidification of Au 49 Ag 5:5 Pd 2:3 Cu 26:9 Si 16:3 bulk metallic glass under various strain rates. Using a copper mold casting technique with a low strain rate during solidification, this alloy is capable of forming glassy rods of at least 5 mm in diameter. Surprisingly, when the liquid alloy is splat cooled at much higher cooling rates and large strain rates, the solidified alloy is no longer fully amorphous. Our finding suggests that the large strain rate during splat cooling induces crystallization. The pronounced difference in crystallization behavior cannot be explained by the previously observed strain rate effect on viscosity alone. A strain rate induced phase separation process is suggested as one of the explanations for this crystallization behavior. The strain-rate-dependent critical cooling rate must be considered in order to assess the intrinsic glass forming ability of metallic liquid. DOI: 10.1103/PhysRevLett.96.075503 PACS numbers: 61.43.Dq, 64.70.Dv, 64.75.+g, 82.60.Lf In the 1950s, Turnbull predicted that glass formation in metals is possible if heterogeneous nucleation could be suppressed [1]. Shortly after, Duwez and co-workers reported the synthesis of the first metallic glass [2] by rapidly cooling an Au-Si alloy at a rate of approximately 10 6 K=s. In the 1970s, ribbons, splats, powder, droplets, wires, and thin films were the typical forms of early metallic glasses obtained by rapid quenching [3,4]. Pd-Cu-Si alloy system was the first exception -Chen's discovery of this alloy system provided the first evidence that metallic glass could be cast in bulk form [5].During the past few decades, bulk metallic glasses have been discovered in a wide range of alloys [6 -11]. In some alloys, a critical cooling rate to avoid crystallization as low as 0:005 K=s [12] and critical casting thickness of up to 7 cm were reported [13] when heterogeneous nucleation was reduced.With the exception of some exotic bulk metallic glass (BMG) synthesis methods [14 -17], most amorphous alloys have been created by cooling the liquid from above its liquidus temperature. In this case, the intrinsic glassforming ability (GFA) and critical casting thickness, d max , were understood to be completely characterized by the critical cooling rate, R c (see, e.g., [18].)This Letter presents solidification studies on gold bulk metallic glass-forming alloy Au 49 Ag 5:5 Pd 2:3 Cu 26:9 Si 16:3 , which could be cast into fully amorphous rods of at least 5 mm in diameter using a conventional copper mold injection method. When the liquid alloy was splat cooled, where it was exposed to both high cooling rate and high strain rate, it crystallized during solidification. This suggests that the high strain rate induces crystallization. This effect becomes less pronounced with increasing processing temperature.Ingots of Au 49 Ag 5:5 Pd 2:3 Cu 26:9 Si 16:3 alloy were prepared by arc-melting the elements (purity: Au, 99.95%; Cu, 99.9%; Ag, 99.5%; Pd, 99.95%; Si, 99.95%) in a titaniumgettered, argon-filled atmosphere. Fu...