Molecular‐Scale Imaging of Water Near Charged Surfaces

Mehlhorn, Michael; Schnur, Sebastian; Groß, Axel; Morgenstern, Karina

doi:10.1002/celc.201300063

Cited by 14 publications

(15 citation statements)

References 38 publications

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“…In the search for greater understanding of ice nucleation processes, we are faced with an unassailable challenge: that the surface sites within which nucleation occurs are only a few nanometers in size. This is much too small to observe the process directly with any presently known experimental techniques, although microscopists continue to make strides in the molecular imaging of ice and of transient phenomena, which may one day lead us to that goal ( 38 , 39 ). However, for now, we are forced to glean knowledge of the mechanism of nucleation indirectly, through the study of the crystals which result from it.…”

Section: Discussionmentioning

confidence: 99%

Active sites for ice nucleation differ depending on nucleation mode

Holden

Campbell

Meldrum

et al. 2021

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

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The nucleation of ice crystals in clouds is poorly understood, despite being of critical importance for our planet’s climate. Nucleation occurs largely at rare “active sites” present on airborne particles such as mineral dust, but the nucleation pathway is distinct under different meteorological conditions. These give rise to two key nucleation pathways where a particle is either immersed in a supercooled liquid water droplet (immersion freezing mode) or suspended in a supersaturated vapor (deposition mode). However, it is unclear if the same active sites are responsible for nucleation in these two modes. Here, we directly compare the sites that are active in these two modes by performing immersion freezing and deposition experiments on the same thin sections of two atmospherically important minerals (feldspar and quartz). For both substrates, we confirm that nucleation is dominated by a limited number of sites and show that there is little correlation between the two sets of sites operating in each experimental method: across both materials, only six out of 73 sites active for immersion freezing nucleation were also active for deposition nucleation. Clearly, different properties determine the activity of nucleation sites for each mode, and we use the pore condensation and freezing concept to argue that effective deposition sites have size and/or geometry requirements not of relevance to effective immersion freezing sites. Hence, the ability to nucleate is pathway dependent, and the mode of nucleation has to be explicitly considered when applying experimental data in cloud models.

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Section: Discussionmentioning

confidence: 99%

Active sites for ice nucleation differ depending on nucleation mode

Holden

Campbell

Meldrum

et al. 2021

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

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“…Another prime candidate for application of this model is two-dimensional ice. It was possible to grow an ice mono-layer 44 to a bi-layer and a multi-layer 45 on a Ru or a Cu surface. Theoretically, the bi-layer ice was previously simulated with molecular dynamics within confinement.…”

Section: Discussionmentioning

confidence: 99%

Modelling the atomic arrangement of amorphous 2D silica: a network analysis

Roy¹,

Heyde

Heuer

2018

Phys. Chem. Chem. Phys.

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The recent experimental discovery of a semi two-dimensional silica glass has offered a realistic description of the random network theory of a silica glass structure, initially discussed by Zachariasen. To study the structure formation of silica in two dimensions, we introduce a two-body force field, based on a soft core Yukawa potential. The different configurations, sampled via Molecular dynamics simulations, can be directly compared with the experimental structures, which have been provided in the literature. The parameters of the force field are obtained from comparison of the nearest-neighbor distances between experiment and simulation. Further key properties such as angle distributions, distribution of ring sizes and triplets of rings are analyzed and compared with the experiment. Of particular interest is the spatial correlation of ring sizes. In general, we observe a very good agreement between experiment and simulation. Additional insight from the simulations is provided about the temporal and spatial stability of the rings in dependence of their size.

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“…Water in the vicinity of hydrophobic and hydrophilic sites of the protein exhibits a dynamical behavior which is quite distinct when compared to bulk water. [20][21][22][23][24][25][26][27] Recently, experiments and simulations with water at the GFP and CYP proteins showed that water molecules at the biomolecule surface present a very slow dynamics and they get stuck in some places, suggesting the presence of fractal traps on the protein surface. 28,29 In these systems, the water near the protein exhibits a subdiffusive behavior in which the mean squared displacement (MSD) of the molecules grows nonlinearly with time, i.e., ⟨r 2 (t)⟩∝ t µ , in which µ < 1 for subdiffusion.…”

Section: Introductionmentioning

confidence: 99%

Dynamical aspects of supercooled TIP3P–water in the grooves of DNA

Santos

Habitzreuter

Schwade

et al. 2019

The Journal of Chemical Physics

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We investigate by molecular dynamics simulations the mobility of the water located at the DNA minor and major grooves. We employ the TIP3P water model, and our system is analyzed for a range of temperatures 190-300 K. For high temperatures, the water at the grooves shows an Arrhenius behavior similar to that observed in the bulk water. At lower temperatures, a departure from the bulk behavior is observed. This slowing down in the dynamics is compared with the dynamics of the hydrogen of the DNA at the grooves and with the autocorrelation functions of the water hydrogen bonds. Our results indicate that the hydrogen bonds of the water at the minor grooves are highly correlated, which suggests that this is the mechanism for the slow dynamics at this high confinement.

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Molecular‐Scale Imaging of Water Near Charged Surfaces

Cited by 14 publications

References 38 publications

Active sites for ice nucleation differ depending on nucleation mode

Active sites for ice nucleation differ depending on nucleation mode

Modelling the atomic arrangement of amorphous 2D silica: a network analysis

Dynamical aspects of supercooled TIP3P–water in the grooves of DNA

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