title: Onset of Cooperative Dynamics in an Equilibrium Glass-Forming Metallic Liquid.
abstract: Onset of cooperative dynamics has been observed in many molecular liquids, colloids, and granular materials in the metastable regime on approaching their respective glass or jamming transition points, and is considered to play a significant role in the emergence of the slow dynamics. However, the nature of such dynamical cooperativity remains elusive in multicomponent metallic liquids characterized by complex many-body interactions and high mixing entropy. Herein, we report evidence of onset of cooperative dynamics in an equilibrium glass-forming metallic liquid (LM601: Zr51Cu36Ni4Al9). This is revealed by deviation of the mean effective diffusion coefficient from its high-temperature Arrhenius behavior below TA ≈ 1300 K, i.e., a crossover from uncorrelated dynamics above TA to landscape-influenced correlated dynamics below TA. Furthermore, the onset/crossover temperature TA in such a multicomponent bulk metallic glass-forming liquid is observed at approximately twice of its calorimetric glass transition temperature (Tg ≈ 697 K) and in its stable liquid phase, unlike many molecular liquids.
authors.affiliation: Department of Nuclear, Plasma and Radiological Engineering, University of Illinois at Urbana-Champaign , Urbana, Illinois 61801, United States.
authors.forename: Abhishek
authors.initials: A
authors.lastname: Jaiswal
authors.affiliation: Liquidmetal Technologies Inc. , Santa Margarita, California 92688, United States.
authors.forename: Stephanie
authors.initials: S
authors.lastname: O'Keeffe
authors.affiliation: Quantum Condensed Matter Division, Oak Ridge National Laboratory , Oak Ridge, Tennessee 37831, United States.
authors.forename: Rebecca
authors.initials: R
authors.lastname: Mills
authors.affiliation: Quantum Condensed Matter Division, Oak Ridge National Laboratory , Oak Ridge, Tennessee 37831, United States.
authors.forename: Andrey
authors.initials: A
authors.lastname: Podlesynak
authors.affiliation: Quantum Condensed Matter Division, Oak Ridge National Laboratory , Oak Ridge, Tennessee 37831, United States.
authors.forename: Georg
authors.initials: G
authors.lastname: Ehlers
authors.affiliation: Department of Materials Science and Engineering, Department of Physics and Astronomy, University of Tennessee , Knoxville, Tennessee 37996, United States.
authors.forename: Wojciech
authors.initials: W
authors.lastname: Dmowski
authors.affiliation: Department of Materials Science and Engineering, Department of Physics and Astronomy, University of Tennessee , Knoxville, Tennessee 37996, United States.
authors.forename: Konstantin
authors.initials: K
authors.lastname: Lokshin
authors.affiliation: Liquidmetal Technologies Inc. , Santa Margarita, California 92688, United States.
authors.forename: Joseph
authors.initials: J
authors.lastname: Stevick
authors.affiliation: Department of Materials Science and Engineering, Department of Physics and Astronomy, University of Tennessee , Knoxville, Tennessee 37996, United States.
authors.forename: Takeshi
authors.initials: T
authors.lastname: Egami
authors.affiliation: Department of Nuclear, Plasma and Radiological Engineering, University of Illinois at Urbana-Champaign , Urbana, Illinois 61801, United States.|Department of Materials Science and Engineering, University of Illinois at Urbana-Champaign , Urbana, Illinois 61801, United States.
authors.forename: Yang
authors.initials: Y
authors.lastname: Zhang