Limits of metastability in amorphous ices: 2H-NMR relaxation

Abstract

The high-frequency reorientation dynamics of O–²H bonds is investigated in various amorphous ices including eHDA (expanded high density amorphous ice), LDA-II (low density amorphous ice II) and HGW (hyperquenched glassy water) using ²H-NMR spin–lattice relaxation as a local probe. Both low density forms, HGW and LDA-II, show similar spin–lattice relaxation but differ in the thermal stability with respect to the transition into crystalline cubic ice I_c. HGW already transforms slightly above 135 K whereas LDA-II crystallizes at 150 K. eHDA is distinguishable from other high density amorphous ices in its thermal stability and spin–lattice relaxation. Its relaxation times are much larger compared to those of VHDA (very high density amorphous ice) and uHDA (unrelaxed high density amorphous ice). eHDA does not show annealing effects, transforms sharply into LDA-II above 123 K and provides higher thermal stability as compared to other high density forms.