Ice crystallization observed in highly supercooled confined water

Stefanutti, E.; Bove, L. E.; Lelong, Gérald; Ricci, Maria Antonietta; Soper, A. K.; Bruni, Fabio

doi:10.1039/c8cp07585a

Cited by 17 publications

(21 citation statements)

References 58 publications

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“…The obtained results are in agreement with other studies reported in the literature for supercooled confined water (Soper, 2008(Soper, , 2012(Soper, , 2013. Stefanutti et al (2019) studied the state of supercooled water confined in MCM-41 using neutron scattering. They have shown the coexistence of freezable pore water with a layer of non-freezable pore water by analysing the change in the Bragg peak intensities.…”

Section: Total X-ray Scatteringsupporting

confidence: 91%

X-ray scattering study of water confined in bioactive glasses: experimental and simulated pair distribution function

et al. 2020

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Temperature-dependent total X-ray scattering measurements for water confined in bioactive glass samples with 5.9 nm pore diameter have been performed. Based on these experimental data, simulations were carried out using the Empirical Potential Structure Refinement (EPSR) code, in order to study the structural organization of the confined water in detail. The results indicate a non-homogeneous structure for water inside the pore, with three different structural organizations of water, depending on the distance from the pore surface: (i) a first layer (4 Å) of interfacial pore water that forms a strong chemical bond with the substrate, (ii) intermediate pore water forming a second layer (4–11 Å) on top of the interfacial pore water, (iii) bulk-like pore water in the centre of the pores. Analysis of the simulated site–site partial pair distribution function shows that the water–silica (Ow–Si) pair correlations occur at ∼3.75 Å. The tetrahedral network of bulk water with oxygen–oxygen (Ow–Ow) hydrogen-bonded pair correlations at ∼2.8, ∼4.1 and ∼4.5 Å is strongly distorted for the interfacial pore water while the second neighbour pair correlations are observed at ∼4.0 and ∼4.9 Å. For the interfacial pore water, an additional Ow–Ow pair correlation appears at ∼3.3 Å, which is likely caused by distortions due to the interactions of the water molecules with the silica at the pore surface.

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Section: Total X-ray Scatteringsupporting

confidence: 91%

X-ray scattering study of water confined in bioactive glasses: experimental and simulated pair distribution function

et al. 2020

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“…This confinement effect is due to the decrease of the probability of molecules near the wall to escape the cage created by the molecules surrounding them, as part of their cage is created by the pore wall and thus never opens. Notice that, this well established confinement effect [34][35][36][37][38][39][40][41][42][43], displays a number of similarities with the effect of a decrease in temperature in supercooled liquids. As expected, when the motor activates the medium in Figures 4b to 4d, the diffusion inside the pores increases.…”

Section: Resultsmentioning

confidence: 99%

“…Confinement of the liquid inside nano-pores has been seen as a way to cutoff the correlation lengths and obtain indirect informations on them by studying the associated dynamical modifications in the liquid. For that fondamental reason as well as multiple practical applications, confinement has been the subject of a number of studies and is still a subject of active research [3,[28][29][30][31][32][33][34][35][36][37][38][39][40][41][42][43]. Indeed, in supercooled liquids, confinement induces various effects.…”

Section: Introductionmentioning

confidence: 99%

Activation of a supercooled liquid confined in a nanopore

Mercier,

Delhaye,

Teboul

2021

Preprint

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It is well stablished that confinement of supercooled liquids in nano-pores induces various effects as a strong modification of the dynamics and a layering of the local structure. In this work we raise the issue as how these confinement effects are modified when the liquid is out of equilibrium. To answer that question, we use molecular dynamics simulations to investigate the effect of confinement on a supercooled liquid activated by the periodic folding of a molecular motor. We find that the motor's opening angle controls the activation of the medium and use that result to study the effect of different activations on the confined supercooled liquid. We observe an increase of the activation effect on the dynamics when the medium is confined. We find that the confinement slowing down dependence with the pore radius depends on the activation of the liquid. We argue that these findings result from a modification of dynamic correlation lengths with activation. In this picture the activation permits to control the liquid correlation length and dynamics inside the pore. Studying the local structure we observe a modification of the layering organization induced by the activation. We also find that the mobility inside the pore depends on the layers, being larger where the local density is small.

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“…However, these ice Bragg peaks appear when h is above 0.4. We note that these Bragg peaks are rather narrow, which indicate that they result from bulk crystals instead of nanometer sized crystals, as the latter will significantly broaden the peaks as seen in [71][72][73][74] . This is further supported by DSC measurement, where no first-order transition is observed at h = 0.3, but it appears at higher hydration levels, h = 0.4 or above.…”

Section: Experimental Evidencementioning

confidence: 87%

The $ω^3$ scaling of the vibrational density of states in quasi-2D nanoconfined solids

Yu,

Yang,

Baggioli

et al. 2021

Preprint

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Atomic vibrations play a vital role in the functions of various physical, chemical, and biological materials. The vibrational properties and the specific heat of a bulk material are well described by the Debye theory, which successfully predicts the quadratic ω 2 low-frequency scaling of the vibrational density of states (VDOS) in bulk solids from few fundamental assumptions. However, the corresponding relationships for nanoconfined materials with fewer degrees of freedom have been far less well explored. In this work, using inelastic neutron scattering, we characterize the VDOS of amorphous ice confined to a thickness of ≈ 1 nm inside graphene oxide membranes and we observe a crossover from the Debye ω 2 scaling to a novel and anomalous ω 3 behaviour upon reducing the confinement size L. Additionally, using molecular dynamics simulations, we not only confirm the experimental findings but also prove that such a novel scaling of the VDOS appears in both crystalline and amorphous solids under slab-confinement. Finally, we theoretically demonstrate that this low-frequency ω 3 law results from the geometric constraints on the momentum phase space induced by confinement along one spatial direction. This new physical phenomenon, revealed by combining theoretical, experimental and simulations results, is relevant to a myriad of systems both in synthetic and biological contexts and it could impact various technological applications for systems under confinement such as nano-devices or thin films.

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Ice crystallization observed in highly supercooled confined water

Abstract: We investigate the state of water confined in the cylindrical pores of MCM-41 type mesoporous silica, with pore diameters of 2.8 nm and 4.5 nm, over the temperature range 160–290 K by combining small angle neutron scattering and wide angle diffraction.

Cited by 17 publications

References 58 publications

X-ray scattering study of water confined in bioactive glasses: experimental and simulated pair distribution function

X-ray scattering study of water confined in bioactive glasses: experimental and simulated pair distribution function

Activation of a supercooled liquid confined in a nanopore

The $ω^3$ scaling of the vibrational density of states in quasi-2D nanoconfined solids

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