The richness of the phase diagram of water reduces drastically at very high pressures where only two molecular phases, protondisordered ice VII and proton-ordered ice VIII, are known. Both phases transform to the centered hydrogen bond atomic phase ice X above about 60 GPa, i.e., at pressures experienced in the interior of large ice bodies in the universe, such as Saturn and Neptune, where nonmolecular ice is thought to be the most abundant phase of water. In this work, we investigate, by Raman spectroscopy up to megabar pressures and ab initio simulations, how the transformation of ice VII in ice X is affected by the presence of salt inclusions in the ice lattice. Considerable amounts of salt can be included in ice VII structure under pressure via rock-ice interaction at depth and processes occurring during planetary accretion. Our study reveals that the presence of salt hinders proton order and hydrogen bond symmetrization, and pushes ice VII to ice X transformation to higher and higher pressures as the concentration of salt is increased.salty ices | extreme conditions | ice bodies | H-bond symmetrization | proton quantum effects A ll models of the interior of ice bodies in the universe rely on our knowledge of the behavior of a few simple molecules under high pressure and temperature (1-22), water being the most intriguing of them, due to its abundance and its connection to life existence.New data delivered by various space missions, such as the Voyager, Galileo, and Cassini-Huygens missions, have greatly improved our understanding of the icy bodies within the solar system (23-25), and recent discoveries of extrasolar planets with significant water ice content have highlighted the importance of high-pressure H 2 O-rich phases in planetary physics beyond the solar system (26).Water displays an unusually rich pressure-temperature phase diagram, which mainly derives from the open geometry of the water molecule, which favors tetrahedral arrangements, and from the possibility of configurational disorder of the protons in the lattice. However, at high pressure (above about 2 GPa), the system experiences a large densification as a result of the interpenetration of low-pressure structures, and only two molecular phases are known, ice VIII and VII (3, 4). Ice VII is composed of two interpenetrating but not interconnected tetrahedral hydrogen-bonded networks of water molecules of normal cubic ice, Ic, with a body-centered-cubic (bcc) oxygen structure. The orientation of the water molecules is disordered, resulting in a paraelectric phase. In the antiferroelectric ice VIII phase, the water molecules and the associated dipole moments on the two sublattices possess long-range order and point in opposite directions, promoting a slight tetragonal distortion of the cubic unit cell along the staggered polarization (3, 4). In these two phases, the hydrogen bonds are characterized by a pronounced double-well proton transfer potential. Upon reducing the distance between donor and acceptor oxygens, the proton potential degenerate...
We studied effective connectivity in rat cortical cultures with various degrees of spatial aggregation, ranging from homogeneous networks to highly aggregated ones. We considered small cultures 3 mm in diameter and that contained about 2000 neurons. Spatial inhomogeneity favored an increase of metric correlations and connectivity among neighboring neurons. Effective connectivity was determined from spontaneous activity recordings using calcium fluorescence imaging. We used generalized transfer entropy as tool to infer the effective connectivity. We carried out numerical simulations to build networks that mimicked the experimental ones and to test the reliability of the connectivity-inference algorithm. Effective connectivity traits were investigated during the development of the cultures over two weeks, and along the gradual blockade of excitatory connections through CNQX. We observed that the average effective connectivity rapidly increased during culture development. At DIV 15 the average excitatory in-degree was measured ask in E 50 for homogeneous and semi aggregated networks, andk in E 120 for aggregated ones, and with 20% inhibition. Aggregated cultures exhibited assortative traits and a high resilience to chemical damage, while the other cultures were dissassortative or neutral, and less resilient. Our work illustrates the role of metric correlations in spatially embedded networks in shaping connectivity and activity traits in living neuronal networks.
It has been known for decades that certain aqueous salt solutions of LiCl and LiBr readily form glasses when cooled to below ≈160 K. This fact has recently been exploited to produce a « salty » high-pressure ice form: When the glass is compressed at low temperatures to pressures higher than 4 GPa and subsequently warmed, it crystallizes into ice VII with the ionic species trapped inside the ice lattice. Here we report the extreme limit of salt incorporation into ice VII, using high pressure neutron diffraction and molecular dynamics simulations. We show that high-pressure crystallisation of aqueous solutions of LiCl∙RH2O and LiBr∙RH2O with R = 5.6 leads to solids with strongly expanded volume, a destruction of the hydrogen-bond network with an isotropic distribution of water-dipole moments, as well as a crystal-to-amorphous transition on decompression. This highly unusual behaviour constitutes an interesting pathway from a glass to a crystal where translational periodicity is restored but the rotational degrees of freedom remaining completely random.
Neural progenitor cells generated from human induced pluripotent stem cells (hiPSCs) are the forefront of ″brain-on-chip″ investigations. Viable and functional hiPSC-derived neuronal networks are shaping powerful in vitro models for evaluating the normal and abnormal formation of cortical circuits, understanding the underlying disease mechanisms, and investigating the response to drugs. They therefore represent a desirable instrument for both the scientific community and the pharmacological industry. However, culture conditions required for the full functional maturation of individual neurons and networks are still unidentified. It has been recognized that three-dimensional (3D) culture conditions can better emulate in vivo neuronal tissue development compared to 2D cultures and thus provide a more desirable in vitro approach. In this paper, we present the design and implementation of a 3D scaffold platform that supports and promotes intricate neuronal network development. 3D scaffolds were produced through direct laser writing by two-photon polymerization (2PP), a high-resolution 3D laser microstructuring technology, using the biocompatible and nondegradable photoreactive resin Dental LT Clear (DClear). Neurons developed and interconnected on a 3D environment shaped by vertically stacked scaffold layers. The developed networks could support different cell types. Starting at the day 50 of 3D culture, neuronal progenitor cells could develop into cortical projection neurons (CNPs) of all six layers, different types of inhibitory neurons, and glia. Additionally and in contrast to 2D conditions, 3D scaffolds supported the long-term culturing of neuronal networks over the course of 120 days. Network health and functionality were probed through calcium imaging, which revealed a strong spontaneous neuronal activity that combined individual and collective events. Taken together, our results highlight advanced microstructured 3D scaffolds as a reliable platform for the 3D in vitro modeling of neuronal functions.
The high density amorphous solution NaCl·10.2D2O crystallises at 260 K as almost pure ice VII during annealing at gigapascal pressures.
Structural characterization of eutectic aqueous NaCl solutions under variable temperature and pressure conditions †The structure of amorphous NaCl solutions produced by fast quenching is studied as a function of pressure, up to 4 GPa, by combined neutron diffraction experiments and classical molecular dynamics simulations. Similarly to LiCl solutions the system amorphizes at ambient pressure in a dense phase structurally similar to the e-HDA phase in pure water. The measurement of the static structure factor as a function of pressure allowed us to validate a new polarizable force field developed by Tazi et al., 2012, never tested under non-ambient conditions.We infer from simulations that the hydration shells of Na + cations form well defined octahedra composed of both H 2 O molecules and Cl À anions at low pressure. These octahedra are gradually broken by the seventh neighbour moving into the shell of first neighbours yielding an irregular geometry. In contrast to LiCl solutions and pure water, the system does not show a polyamorphic transition under pressure. This confirms that the existence of polyamorphism relies on the tetrahedral structure of water molecules, which is broken here.
Scaffolds and patterned substrates are among the most successful strategies to dictate the connectivity between neurons in culture. Here, we used numerical simulations to investigate the capacity of physical obstacles placed on a flat substrate to shape structural connectivity, and in turn collective dynamics and effective connectivity, in biologically-realistic neuronal networks. We considered μ-sized obstacles placed in mm-sized networks. Three main obstacle shapes were explored, namely crosses, circles and triangles of isosceles profile. They occupied either a small area fraction of the substrate or populated it entirely in a periodic manner. From the point of view of structure, all obstacles promoted short length-scale connections, shifted the in- and out-degree distributions toward lower values, and increased the modularity of the networks. The capacity of obstacles to shape distinct structural traits depended on their density and the ratio between axonal length and substrate diameter. For high densities, different features were triggered depending on obstacle shape, with crosses trapping axons in their vicinity and triangles funneling axons along the reverse direction of their tip. From the point of view of dynamics, obstacles reduced the capacity of networks to spontaneously activate, with triangles in turn strongly dictating the direction of activity propagation. Effective connectivity networks, inferred using transfer entropy, exhibited distinct modular traits, indicating that the presence of obstacles facilitated the formation of local effective microcircuits. Our study illustrates the potential of physical constraints to shape structural blueprints and remodel collective activity, and may guide investigations aimed at mimicking organizational traits of biological neuronal circuits.
We identified photopolymers for 2-photon polymerisation with biocompatibility for human iPSC-derived neural network development. Generation of microscale scaffold topologies enabled neurite guidance, demonstrating use in reproducing aligned networks.
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