Long-Range Mass Transport during Structural Transitions in Metallic Glass-Forming Melts

We investigate the structure and dynamics of the bulk metallic glass-forming alloys Zr_{41.2}Ti_{13.8}Cu_{12.5}Ni_{10}Be_{22.5} and Zr_{58.5}Cu_{15.6}Ni_{12.8}Al_{10.3}Nb_{2.8}. Combining in situ synchrotron x-ray diffraction and quasielastic neutron scattering with electrostatic levitation, we directly observe an abrupt change in the temperature dependence of the first structure factor maximum of these melts. We find that the kinetics of this liquid-liquid transition during cooling are on the order of tens of seconds, whereas its onset temperature depends only weakly on the applied cooling rate. Such slow transition kinetics require long-range mass transport, which is incompatible with a transition mechanism involving only local structural changes as in oxides or molecular liquids.