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Title: First-Order Phase Transition in Liquid Ag to the Heterogenous G-Phase
A molten metal is an atomic liquid that lacks directional bonding and is free from chemical ordering effects. Experimentally, liquid metals can be undercooled by up to ∼20% of their melting temperature but crystallize rapidly in subnanosecond time scales at deeper undercooling. To address this limited metastability with respect to crystallization, we employed molecular dynamics simulations to study the thermodynamics and kinetics of the glass transition and crystallization in deeply undercooled liquid Ag. We present direct evidence that undercooled liquid Ag undergoes a first-order configurational freezing transition from the high-temperature homogeneous disordered liquid phase (L) to a metastable, heterogeneous, configura-tionally ordered state that displays elastic rigidity with a persistent and finite shear modulus, μ. We designate this ordered state as the G-phase and conclude it is a metastable non-crystalline phase. We show that the L−G transition occurs by nucleation of the G-phase from the L-phase. Both te L- and G-phases are metastable because both ultimately crystallize. The observed first-order transition is reversible: the G-phase displays a first-order melting transition to the L-phase at a coexistence temperature, TG,M. We develop a thermodynamic description of the two phases and their coexistence boundary.  more » « less
Award ID(s):
1710744
PAR ID:
10139158
Author(s) / Creator(s):
; ; ; ;
Date Published:
Journal Name:
The journal of physical chemistry letters
Volume:
11
ISSN:
1948-7185
Page Range / eLocation ID:
632-645
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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