Water shows unusual behavior when it is supercooled, i.e., changes in compressibility, heat capacity, and the thermal expansion coefficient. One explanation for some of this behavior is a liquid-liquid transition between a high-density liquid and a low-density liquid, with a liquid-liquid critical point at supercooled temperatures. However, studying these phenomena experimentally is challenging due to the tendency of supercooled water to crystallize.
Anders Nilsson, Stockholm University, Sweden, and colleagues have found experimental evidence for a liquid-liquid transition in bulk supercooled water using a compression-expansion procedure. The team used an infrared femtosecond laser to heat high-density amorphous ice and create bulk samples of supercooled liquid water under pressure. This first results in a high-density liquid phase, which then expands. The researchers studied the changes in the water’s structure during the expansion using femtosecond X-ray laser pulses. This ultrafast structure determination allowed them to observe structural changes before the water crystallized again.
The team estimates that the initial pressure in the high-density liquid phase is 2.5–3.5 kbar before the rapid expansion. They found that within 20 ns–3 μs, low-density liquid domains appeared and grew, which caused changes in the observed x-ray scattering intensity. Crystallization of the supercooled samples was slower and occurred on time scales of 3–50 μs. According to the researchers, this work supports the existence of a liquid-liquid critical point in water and could help with finding its exact location.
- Experimental observation of the liquid-liquid transition in bulk supercooled water under pressure,
Kyung Hwan Kim, Katrin Amann-Winkel, Nicolas Giovambattista, Alexander Späh, Fivos Perakis, Harshad Pathak, Marjorie Ladd Parada, Cheolhee Yang, Daniel Mariedahl, Tobias Eklund, Thomas. J. Lane, Seonju You, Sangmin Jeong, Matthew Weston, Jae Hyuk Lee, Intae Eom, Minseok Kim, Jaeku Park, Sae Hwan Chun, Peter H. Poole, Anders Nilsson,