Bulk Melting of Ice at the Limit of Superheating

Schmeisser, Marcus; Iglev, Hristo; Laubereau, A.

doi:10.1021/jp0736802

Cited by 23 publications

(35 citation statements)

References 37 publications

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“…1B), and the formation of a superheated crystal at T1 > Tm . This T jump is achieved through redistribution of the vibrational energy through the lattice modes (thermalization), completed in ∼20 ps, during which melting already starts (13,16). The estimated pressure change (1.3 MPa·K −1 ) (13) is 50 MPa during the pulse and rapidly decreases due to melting itself in ice I h (9).…”

Section: Resultsmentioning

confidence: 99%

“…The structural changes following the heating pulse have been monitored in aluminum (14) and gold (15) by electron diffraction with a sample thickness of 20 nm, where the main signatures of melting complete in a few picoseconds. Water ice melting after an ultrafast T jump has been studied by time-resolved infrared spectra (13,16), with a sample thickness of 1.6 µm and over a time window of 250 ps. Here, the spectral changes attributed by the authors to melting mostly occur in the first 150 ps after the pulse (τ = 37 ps) (16).…”

mentioning

confidence: 99%

“…Water ice melting after an ultrafast T jump has been studied by time-resolved infrared spectra (13,16), with a sample thickness of 1.6 µm and over a time window of 250 ps. Here, the spectral changes attributed by the authors to melting mostly occur in the first 150 ps after the pulse (τ = 37 ps) (16). At 250 ps an incomplete melting was still observed, consistent with the amount of energy delivered.…”

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confidence: 99%

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Melting dynamics of ice in the mesoscopic regime

Citroni

Fanetti

Falsini³

et al. 2017

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

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How does a crystal melt? How long does it take for melt nuclei to grow? The melting mechanisms have been addressed by several theoretical and experimental works, covering a subnanosecond time window with sample sizes of tens of nanometers and thus suitable to determine the onset of the process but unable to unveil the following dynamics. On the other hand, macroscopic observations of phase transitions, with millisecond or longer time resolution, account for processes occurring at surfaces and time limited by thermal contact with the environment. Here, we fill the gap between these two extremes, investigating the melting of ice in the entire mesoscopic regime. A bulk ice I h or ice VI sample is homogeneously heated by a picosecond infrared pulse, which delivers all of the energy necessary for complete melting. The evolution of melt/ice interfaces thereafter is monitored by Mie scattering with nanosecond resolution, for all of the time needed for the sample to reequilibrate. The growth of the liquid domains, over distances of micrometers, takes hundreds of nanoseconds, a time orders of magnitude larger than expected from simple H-bond dynamics.Mie scattering | temperature jump | superheating | laser heating | anvil cell M elting of ice is one of the most common occurrences on our planet, from polar ices to glaciers, to the morning frost and the preparation of our drinks. Ices are present as well in extraterrestrial environments, planetary and intersellar, going through extremely different pressure and temperature conditions, where many phase boundaries are encountered. The molecular mechanisms of melting and the characteristic timescales of the process are not well elucidated, as for any other phase transition. In fact, great effort is presently being made with state of the art experimental techniques to understand the intrinsic kinetics of structural transformations, particularly under dynamic compression, by which phase-transition boundaries up to extreme pressures (P) and temperatures (T) can be accessed (1-6). Melting is the least hindered of phase transitions, requiring the disruption of the crystalline order and the achievement of the local structure of the liquid phase.The dynamics of melting have been studied up to the present in the picosecond timescale, observing structural changes on a length scale of few nanometers, in the attempt to explain the fundamental mechanisms of the transition onset. In both simulations and experiments, micrometric-or submicrometric-sized crystals can be rapidly heated above the melting temperature (Tm ), into a superheated state where melting occurs. Metals and water ice have been the test systems. Simulations have revealed a nucleation and growth mechanism (7-11), and nucleation has been especially addressed, in trying to determine the minimum number of atoms/molecules needed to form a critical nucleus for the transitions, the solid/melt interfacial energy, the transient local structures achieved during the transformation, and the role of defects and surfaces. Experimentally...

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Section: Resultsmentioning

confidence: 99%

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confidence: 99%

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confidence: 99%

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Melting dynamics of ice in the mesoscopic regime

Citroni

Fanetti

Falsini³

et al. 2017

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

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“…Also, for crystals that are surrounded by a gas or solid, surface melting is known to occur even at temperatures below the bulk melting point (i.e., premelting) (5). Nevertheless, recent studies demonstrate that solids can be superheated if surface melting is circumvented (4,(6)(7)(8)(9). For example, high superheating values were achieved by embedding nanocrystals of one substance into another material with a higher melting point (4,8).…”

Section: Gibbs-thomson Effect | Ice Recrystallization | Irreversible mentioning

confidence: 99%

Superheating of ice crystals in antifreeze protein solutions

Celik

Graham

Mok

et al. 2010

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

128

126

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It has been argued that for antifreeze proteins (AFPs) to stop ice crystal growth, they must irreversibly bind to the ice surface. Surface-adsorbed AFPs should also prevent ice from melting, but to date this has been demonstrated only in a qualitative manner. Here we present the first quantitative measurements of superheating of ice in AFP solutions. Superheated ice crystals were stable for hours above their equilibrium melting point, and the maximum superheating obtained was 0.44°C. When melting commenced in this superheated regime, rapid melting of the crystals from a point on the surface was observed. This increase in melting temperature was more appreciable for hyperactive AFPs compared to the AFPs with moderate antifreeze activity. For each of the AFP solutions that exhibited superheating, the enhancement of the melting temperature was far smaller than the depression of the freezing temperature. The present findings clearly show that AFPs adsorb to ice surfaces as part of their mechanism of action, and this absorption leads to protection of ice against melting as well as freezing.Gibbs-Thomson effect | ice recrystallization | irreversible binding | melting hysteresis | thermal hysteresis

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“…We have no evidence that the kinetics may be governed by other mechanistic reasons such as reported for phase transitions in ice by the group of Laubereau. 75 Fig . 4 shows time-resolved photoelectron spectra of methanol heated to a temperature of about 550 AE 100 K. Similar to water, the photoelectron spectra of methanol also consist of a superposition of the liquid and the gas phase photoelectron emission lines.…”

Section: Resultsmentioning

confidence: 99%

Hydrogen bond dynamics of superheated water and methanol by ultrafast IR-pump and EUV-photoelectron probe spectroscopy

Vöhringer‐Martinez

Link

Lugovoy

et al. 2014

Phys. Chem. Chem. Phys.

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Supercritical water and methanol have recently drawn much attention in the field of green chemistry. It is crucial to an understanding of supercritical solvents to know their dynamics and to what extent hydrogen (H) bonds persist in these fluids. Here, we show that with femtosecond infrared (IR) laser pulses water and methanol can be heated to temperatures near and above their critical temperature T c and their molecular dynamics can be studied via ultrafast photoelectron spectroscopy at liquid jet interfaces with high harmonics radiation. As opposed to previous studies, the main focus here is the comparison between the hydrogen bonded systems of methanol and water and their interpretation by theory. Superheated water initially forms a dense hot phase with spectral features resembling those of monomers in gas phase water. On longer timescales, this phase was found to build hot aggregates, whose size increases as a function of time. In contrast, methanol heated to temperatures near T c initially forms a broad distribution of aggregate sizes and some gas. These experimental features are also found and analyzed in extended molecular dynamics simulations. Additionally, the simulations enabled us to relate the origin of the different behavior of these two hydrogen-bonded liquids to the nature of the intermolecular potentials. The combined experimental and theoretical approach delivers new insights into both superheated phases and may contribute to understand their different chemical reactivities.

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Bulk Melting of Ice at the Limit of Superheating

Cited by 23 publications

References 37 publications

Melting dynamics of ice in the mesoscopic regime

Melting dynamics of ice in the mesoscopic regime

Superheating of ice crystals in antifreeze protein solutions

Hydrogen bond dynamics of superheated water and methanol by ultrafast IR-pump and EUV-photoelectron probe spectroscopy

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