Reflection high energy electron diffraction (RHEED) study of ice nucleation and growth on Ni(111): influences of adspecies and electron irradiation

Abstract

How interfacial molecular interactions influence nucleation and growth processes of water ice is explored using pristine, oxygenated, and CO-adsorbed Ni(111) substrates based on RHEED, together with the effects of high-energy electron irradiation on the crystallization kinetics. A monolayer of amorphous solid water deposited onto the pristine Ni(111) substrate crystallizes into ice Ic at ca. 150 K, whereas ice Ih (Ic) is formed preferentially during water vapor deposition at 135 K (125 K). The ice nucleation tends to be hampered on the oxygenated Ni(111) surface because of the hydrogen bond formation with chemisorbed oxygen, leading to the growth of randomly-oriented ice Ic crystallites via spontaneous nucleation. The amorphization and recrystallization of initially crystalline ices are observed during prolonged RHEED measurements at 20 and 70 K, respectively, signifying that high-energy electron irradiation has both thermal and non-thermal effects on the water phase transition. The epitaxial growth (non-epitaxial growth) of ice occurs during electron irradiation of amorphous solid water formed on the pristine and oxygenated Ni(111) substrates (CO-adsorbed Ni(111) substrate) even at 100 K (120 K) because nucleation and growth are initiated at the substrate interface (in the ASW film interior).