Fast dynamics and high effective dimensionality of liquid fluidity.

Fluidity, the ability of liquids to flow, is the key property distinguishing liquids from solids. This fluidity is set by the mobile transit atoms moving from one quasi-equilibrium point to the next. The nature of this transit motion is unknown. Here, we show that flow-enabling transits form a dynamically distinct sub-ensemble where atoms move on average faster than the overall system, with a manifestly non-Maxwellian velocity distribution. This is in contrast to solids and gases where no distinction of different ensembles can be made and where the distribution is always Maxwellian. The non-Maxwellian distribution is described by an exponent [Formula: see text] corresponding to high dimensionality of space. This is generally similar to extra synthetic dimensions in topological quantum matter, albeit higher dimensionality in liquids is not integer but is fractional. The dimensionality is close to 4 at melting and exceeds 4 at high temperature. [Formula: see text] has a maximum as a function of temperature and pressure in liquid and supercritical states, returning to its Maxwell value in the solid and gas states.

Evolution of amorphous structure under irradiation: zircon case study.

The nature of the amorphous state has been notably difficult to ascertain at the microscopic level. In addition to the fundamental importance of understanding the amorphous state, potential changes to amorphous structures as a result of radiation damage have direct implications for the pressing problem of nuclear waste encapsulation. Here, we develop new methods to identify and quantify the damage produced by high-energy collision cascades that are applicable to amorphous structures and perform large-scale molecular dynamics simulations of high-energy collision cascades in a model zircon system. We find that, whereas the averaged probes of order such as pair distribution function do not indicate structural changes, local coordination analysis shows that the amorphous structure substantially evolves due to radiation damage. Our analysis shows a correlation between the local structural changes and enthalpy. Important implications for the long-term storage of nuclear waste follow from our detection of significant local density inhomogeneities. Although we do not reach the point of convergence where the changes of the amorphous structure saturate, our results imply that the nature of this new converged amorphous state will be of substantial interest in future experimental and modeling work.

Pronounced structural crossover in water at supercritical pressures.

There have been ample studies of the many phases of H2O in both its solid and low pressure liquid states, and the transitions between them. Using molecular dynamics simulations we address the hitherto unexplored deeply supercritical pressures, where no qualitative transitions are thought to take place and where all properties are expected to vary smoothly. On the basis of these simulations we predict that water at supercritical pressures undergoes a structural crossover across the Frenkel line at pressures as high as 45 times the critical pressure. This provides a new insight into the water phase diagram and establishes a link between the structural and dynamical properties of supercritical water. Specifically, the crossover is demonstrated by a sharp and pronounced at low pressures, and smooth at high pressures, signified by changes in the pair distribution functions and local coordination which coincide with the dynamical transition (the loss of all oscillatory molecular motion) at the Frenkel line on the phase diagram.