Abstract
We investigate the H/D isotope effect in a liquid-liquid transition in crystallization-resistant supercooled aqueous solution. Using steady-state infrared spectroscopy and measuring thermal conductivities, we observe a ≈5 K shift in the onset temperature of the liquid-liquid transition, a value that is similar to the H/D isotope shifts of the HDA-LDA transition and of the Widom line of pure supercooled water [Kim et al ., Science 358 , 1589 (2017)], and that highlights the importance of isotope effects in water's supercooled regime. By employing multivariate data analysis we find isosbestic point related to the phase transformation in both isotopic systems, indicating phase coexistence during the transition. This article is dedicated to the memory of Austen Angell, and we begin with some personal memories of his two stays at the University of Amsterdam.
Highlights
We investigate the H/D isotope effect in a liquid-liquid transition in crystallization-resistant supercooled aqueous solution
Thermal conductivity measurements and multivariate curve resolution techniques, we investigate the isotope effect in the transition temperature, and we characterize the coexistence of two phases during the transition
We investigate isotope effects related to a liquid-liquid transition (LLT) in supercooled aqueous solutions and its deuterated counterpart by measuring their infrared absorption spectra and thermal conductivities whilst cooling down and reheating in a cryostat
Summary
Austen Angell and the University of Amsterdam have a long history, ranging from his sabbatical year in Amsterdam in 1971 to our joint research in the period 2015–2021 some 50 years later, and of which this article may be regarded as a coda. Fastforward about 50 years: Gerard Wegdam, Rob Bonn and Jan van der Elsken had retired, but Daniel Bonn, son of Rob Bonn, was a professor in Soft Matter physics at the University of Amsterdam. He had met Austen at a conference, and they agreed Austen would visit the UvA, to discuss a potential cooperation, and as a sentimental journey. The compatibility of the hydrogenbond networks of solvent and solute was macroscopically observable as ideal freezing-point depression behavior Austen and his postdoc Zuo feng Zhao had carefully investigated these solutions, and had discovered that they exhibit a first-order like phase transition at very low temper ature. Austen was dear to all of us, and we dedicate this article to his memory
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