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We observe, at low temperature, the appearance of propagating events thatoriginate from the inter-conversion between adjacent four and five coordinatedwater molecules in supercooled liquid water, resulting in the migration of thecoordination number five in a string-like fashion, creating rotational jumpsalong the way. The length of the connected events increases with loweringtemperature. Each propagation event is terminated by a 3-coordinated species,present in a small number at large supercooling, which interacts cooperativelywith 5-coordinated molecules to annihilate both the species. We find that thesegrowing dynamical correlations manifest in a divergent-like growth of anon-linear density response function, \times4(t), which is given by a fourpoint time correlation function (FPTCF). The locus of the maximum of\times4(t), when plotted against the time t* of maximum, exhibits a sharp peakprecisely at the temperature where the static response functions (specificheat, isothermal compressibility) also show similar sharp, divergent-like,peak. While the decay of population fluctuation time correlation function ofboth 4- and 5- coordinated species slows down dramatically and a step-likefeature of the relaxation becomes evident, the lifetime itself of 5-corrdinatedspecies remains short. These results suggest a new molecular mechanism of lowtemperature anomalies and of the liquid-liquid transition in terms ofinitiation, growth and termination of propagating jump and inter-conversionevents.

Propagating rotational jump events drive liquid-liquid transition in supercooled liquid water