Emergence of correlated proton tunnelling in water ice

Proc Math Phys Eng Sci. 2019 May;475(2225):20180867. doi: 10.1098/rspa.2018.0867. Epub 2019 May 15.

Abstract

Several experimental and theoretical studies report instances of concerted or correlated multiple proton tunnelling in solid phases of water. Here, we construct a pseudo-spin model for the quantum motion of protons in a hexameric H2O ring and extend it to open system dynamics that takes environmental effects into account in the form of O-H stretch vibrations. We approach the problem of correlations in tunnelling using quantum information theory in a departure from previous studies. Our formalism enables us to quantify the coherent proton mobility around the hexagonal ring by one of the principal measures of coherence, the l 1 norm of coherence. The nature of the pairwise pseudo-spin correlations underlying the overall mobility is further investigated within this formalism. We show that the classical correlations of the individual quantum tunnelling events in long-time limit is sufficient to capture the behaviour of coherent proton mobility observed in low-temperature experiments. We conclude that long-range intra-ring interactions do not appear to be a necessary condition for correlated proton tunnelling in water ice.

Keywords: low-temperature protontunnelling in water ice; measures of quantum coherence; measures of quantumcorrelations; open quantum systems; quantum information; quantum master equation.

Associated data

  • figshare/10.6084/m9.figshare.c.4487114