TY - JOUR
T1 - Relaxation dynamics and transformation kinetics of deeply supercooled water
T2 - Temperature, pressure, doping, and proton/deuteron isotope effects
AU - Lemke, Sonja
AU - Handle, Philip H.
AU - Plaga, Lucie J.
AU - Stern, Josef N.
AU - Seidl, Markus
AU - Fuentes-Landete, Violeta
AU - Amann-Winkel, Katrin
AU - Köster, Karsten W.
AU - Gainaru, Catalin
AU - Loerting, Thomas
AU - Böhmer, Roland
N1 - Publisher Copyright:
© 2017 Author(s).
PY - 2017/7/21
Y1 - 2017/7/21
N2 - Above its glass transition, the equilibrated high-density amorphous ice (HDA) transforms to the low-density pendant (LDA). The temperature dependence of the transformation is monitored at ambient pressure using dielectric spectroscopy and at elevated pressures using dilatometry. It is found that near the glass transition temperature of deuterated samples, the transformation kinetics is 300 times slower than the structural relaxation, while for protonated samples, the time scale separation is at least 30 000 and insensitive to doping. The kinetics of the HDA to LDA transformation lacks a proton/deuteron isotope effect, revealing that this process is dominated by the restructuring of the oxygen network. The x-ray diffraction experiments performed on samples at intermediate transition stages reflect a linear combination of the LDA and HDA patterns implying a macroscopic phase separation, instead of a local intermixing of the two amorphous states.
AB - Above its glass transition, the equilibrated high-density amorphous ice (HDA) transforms to the low-density pendant (LDA). The temperature dependence of the transformation is monitored at ambient pressure using dielectric spectroscopy and at elevated pressures using dilatometry. It is found that near the glass transition temperature of deuterated samples, the transformation kinetics is 300 times slower than the structural relaxation, while for protonated samples, the time scale separation is at least 30 000 and insensitive to doping. The kinetics of the HDA to LDA transformation lacks a proton/deuteron isotope effect, revealing that this process is dominated by the restructuring of the oxygen network. The x-ray diffraction experiments performed on samples at intermediate transition stages reflect a linear combination of the LDA and HDA patterns implying a macroscopic phase separation, instead of a local intermixing of the two amorphous states.
UR - http://www.scopus.com/inward/record.url?scp=85025170084&partnerID=8YFLogxK
U2 - 10.1063/1.4993790
DO - 10.1063/1.4993790
M3 - Article
C2 - 28734291
AN - SCOPUS:85025170084
SN - 0021-9606
VL - 147
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
IS - 3
M1 - 034506
ER -