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The striking anomalies in physical properties of supercooled water that werediscovered in the 1960-70s, remain incompletely understood and so provide botha source of controversy amongst theoreticians, and a stimulus toexperimentalists and simulators to find new ways of penetrating the"crystallization curtain" that effectively shields the problem from solution.Recently a new door on the problem was opened by showing that, in idealsolutions, made using ionic liquid solutes, water anomalies are not destroyedas earlier found for common salt and most molecular solutes, but instead areenhanced to the point of precipitating an apparently first order liquid-liquidtransition. The evidence was a spike in apparent heat capacity during coolingthat could be fully reversed during reheating before any sign of icecrystallization appeared. Here, we use decoupled-oscillator infraredspectroscopy to define the structural character of this phenomenon usingsimilar down and upscan rates as in the calorimetric study. Thin-film samplesalso permit slow scans (1 K/min) in which the transition has a width of lessthan 1 K, and is fully reversible. The OH spectrum changes discontinuously atthe phase-transition temperature, indicating a discrete change in hydrogen-bondstructure. The spectral changes show that the low-temperature liquid is morestrongly hydrogen bonded and less disordered as compared to thehigh-temperature liquid. The spectrum of the low-temperature liquid isessentially that seen in low-density amorphous water. This similarity suggeststhat the liquid-liquid transition observed here also exists in neat undercooledwater, providing a unified explanation for many of its anomalies.

Liquid-liquid transition in supercooled aqueous solution involving a low-temperature phase similar to low-density amorphous water