Glass transition of aqueous solutions involving annealing-induced ice recrystallization resolves liquid-liquid transition puzzle of water.
Liquid-liquid transition of water is an important concept in condensed-matter physics. Recently, it was claimed to have been confirmed in aqueous solutions based on annealing-induced upshift of glass-liquid transition temperature, T(g) . Here we report a universal water-content, X(aqu) , dependence of T(g) for aqueous solutions. Solutions with X(aqu)>X(cr)(aqu)vitrify/devitrify at a constant temperature, ~T(g) , referring to freeze-concentrated phase with X(aqu)left behind ice crystallization. Those solutions with X(aqu)<X(aqu)<X(cr)(aqu) totally vitrify at Tg<Tg under conventional cooling/heating process though, Tg of the samples annealed at temperatures   to effectively evoke ice recrystallization is stabilized at . Experiments on aqueous glycerol and 1,2,4-butanetriol solutions in literature were repeated, and the same samples subject to other annealing treatments equally reproduce the result. The upshift of T(g) by annealing is attributable to freeze-concentrated phase of solutions instead of 'liquid II phase of water'. Our work also provides a reliable method to determine hydration formula and to scrutinize solute-solvent interaction in solution.
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China.|Department of Physics, University of Science and Technology Beijing, Beijing 100083, China.
Li-Shan
LS
Zhao
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China.
Ze-Xian
ZX
Cao
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China.
Qiang
Q
Wang