Experimental observation of nanophase segregation in aqueous salt solutions around the predicted liquid–liquid transition in water

Lane, Paul D.; Reichenbach, Judith; Farrell, Andrew; Ramakers, Lennart A. I.; Adamczyk, Katrin; Hunt, Neil T.; Wynne, Klaas

doi:10.1039/c9cp06082k

Cited by 7 publications

(7 citation statements)

References 55 publications

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“…This crystallization is a consequence of the nanosegregation of the solution that leads to the formation of small domains of water, a phenomenon that is already visible in the liquid structure near the melting temperature ( 38 ). Nanosegregation of water, and its connection to ice formation, is a more general phenomenon that has also been observed, for instance, in aqueous salt solutions for a range of concentrations ( 39 – 41 ).…”

Section: Resultsmentioning

confidence: 85%

Interplay of vitrification and ice formation in a cryoprotectant aqueous solution at low temperature

Alba‐Simionesco

Judeinstein

Longeville

et al. 2022

Proc. Natl. Acad. Sci. U.S.A.

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Significance Studying water crystallization at low temperature and the lower limit of ice formation is crucial both for a fundamental understanding of water and for practical reasons such as cryopreservation. By taking advantage of the polarized neutron scattering technique and by considering a nanosegregated water–glycerol solution, we are able to characterize the key parameters of ice formation at temperatures near and below the calorimetric glass transition of the solution and provide a general rule for estimating the lower temperature limit of water crystallization in a broad range of aqueous solutions. We also show that nanosegregated water in the glassy solution at low temperature is not in a high-density form but in a low-density one.

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Section: Resultsmentioning

confidence: 85%

Interplay of vitrification and ice formation in a cryoprotectant aqueous solution at low temperature

Alba‐Simionesco

Judeinstein

Longeville

et al. 2022

Proc. Natl. Acad. Sci. U.S.A.

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“…This crystallization is a consequence of the nano-segregation of the solution that leads to the formation of small domains of water, a phenomenon whose premises can already be found in the liquid structure near the melting temperature 35 . Nano-segregation of water, and its connection to ice formation, is a more general phenomenon that has also been observed for instance in aqueous salt solutions for a range of concentrations [36][37][38] .…”

Section: Water Crystallization Near and Below The Calorimetric Glass ...mentioning

confidence: 71%

Interplay of vitrification and ice formation in a cryoprotectant aqueous solution at low temperature

Alba-Simionesco,

Judeinstein,

Longeville

et al. 2021

Preprint

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The proneness of water to crystallize is a major obstacle to understanding its putative exotic behavior in the supercooled state. It also represents a strong practical limitation to cryopreservation of biological systems. Adding some concentration of glycerol, which has a cryoprotective effect preventing to some degree water crystallization, has been proposed as a possible way out, provided the concentration is small enough for water to retain some of its bulk character and/or for limiting the damage caused by glycerol on living organisms. Contrary to previous expectations, we show that in the "marginal" glycerol molar concentration ≈ 18%, at which vitrification is possible with no crystallization on rapid cooling, water crystallizes upon isothermal annealing even below the calorimetric glass transition of the solution. Through a time-resolved polarized neutron scattering investigation, we extract key parameters, size and shape of the ice crystallites, fraction of water that crystallizes, crystallization time, which are important for cryoprotection, as a function of the annealing temperature. We also characterize the nature of the out-of-equilibrium liquid phases that are present at low temperature, providing more arguments against the presence of an isocompositional liquid-liquid transition. Finally, we propose a rule-of-thumb to estimate the lower temperature limit below which water crystallization does not occur in aqueous solutions.

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“…The high-frequency oscillations can be well-modeled using the Brownian oscillator function, 29 , 39 or the antisymmetrized Gaussian (ASG) function, 40 , 41 where ω o and ω G are the undamped oscillator frequencies, γ is the damping rate, and σ G is related to the full width at half-maximum (fwhm) of the Gaussian line shape by . It was found that the fast-β mode was following a Brownian oscillator throughout, whereas librations fit a Brownian for n -alkanes except propane and an antisymmetrized Gaussian otherwise.…”

Section: Methodsmentioning

confidence: 99%

Low-Frequency (Gigahertz to Terahertz) Depolarized Raman Scattering Offn-Alkanes, Cycloalkanes, and Six-Membered Rings: A Physical Interpretation

et al. 2020

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Molecular liquids have long been known to undergo various distinct intermolecular motions, from fast librations and cage-rattling oscillations to slow orientational and translational diffusion. However, their resultant gigahertz to terahertz spectra are far from simple, appearing as broad shapeless bands that span many orders of magnitude of frequency, making meaningful interpretation troublesome. Ad hoc spectral line shape fitting has become a notoriously fine art in the field; a unified approach to handling such spectra is long overdue. Here we apply ultrafast optical Kerr-effect (OKE) spectroscopy to study the intermolecular dynamics of room-temperature n -alkanes, cycloalkanes, and six-carbon rings, as well as liquid methane and propane. This work provides stress tests and converges upon an experimentally robust model across simple molecular series and range of temperatures, providing a blueprint for the interpretation of the dynamics of van der Waals liquids. This will enable the interpretation of low-frequency spectra of more complex liquids.

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Experimental observation of nanophase segregation in aqueous salt solutions around the predicted liquid–liquid transition in water

Abstract: Using ultrafast spectroscopy to determine temperature-dependent structuring of water, solvation of ions and the size of phase segregated domains.

Cited by 7 publications

References 55 publications

Interplay of vitrification and ice formation in a cryoprotectant aqueous solution at low temperature

Interplay of vitrification and ice formation in a cryoprotectant aqueous solution at low temperature

Interplay of vitrification and ice formation in a cryoprotectant aqueous solution at low temperature

Low-Frequency (Gigahertz to Terahertz) Depolarized Raman Scattering Offn-Alkanes, Cycloalkanes, and Six-Membered Rings: A Physical Interpretation

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