Gotowa bibliografia na temat „QUANTUM SUPERCOOLED LIQUID”

The recently developed quantum molecular dynamics method including nuclear quantum effects demonstrated that supercooled hydrogens exhibit intrinsic properties including a precursor of superfluidity which neither normal hydrogen liquid nor solid possesses.

We developed the RexPoN force field for water based entirely on quantum mechanics. It predicts the properties of water extremely accurately, withTmelt= 273.3 K (273.15 K) and properties at 298 K: ΔHvap= 10.36 kcal/mol (10.52), density = 0.9965 g/cm3(0.9965), entropy = 68.4 J/mol/K (69.9), and dielectric constant = 76.1 (78.4), where experimental values are in parentheses. Upon heating from 0.0 K (ice) to 273.0 K (still ice), the average number of strong hydrogen bonds (SHBs, rOO≤ 2.93 Å) decreases from 4.0 to 3.3, but upon melting at 273.5 K, the number of SHBs drops suddenly to 2.3, decreasing slowly to 2.1 at 298 K and 1.6 at 400 K. The lifetime of the SHBs is 90.3 fs at 298 K, increasing monotonically for lower temperature. These SHBs connect to form multibranched polymer chains (151 H2O per chain at 298 K), where branch points have 3 SHBs and termination points have 1 SHB. This dynamic fluctuating branched polymer view of water provides a dramatically modified paradigm for understanding the properties of water. It may explain the 20-nm angular correlation lengths at 298 K and the critical point at 227 K in supercooled water. Indeed, the 15% jump in the SHB lifetime at 227 K suggests that the supercooled critical point may correspond to a phase transition temperature of the dynamic polymer structure. This paradigm for water could have a significant impact on the properties for protein, DNA, and other materials in aqueous media.

The random first order transition theory (RFOT) describing the transition from a supercooled liquid to an ideal glass has been actively developed over the last twenty years. This theory is formulated in a way that allows a description of the transition from the initial equilibrium state to the final metastable state without considering any kinetic processes. The RFOT and its applications for real molecular systems (multicomponent liquids with various intermolecular potentials, gel systems, etc.) are widely represented in English-language sources. However, these studies are practically not described in any Russian sources. This paper presents an overview of the studies carried out in this field. REFERENCES 1. Sanditov D. S., Ojovan M. I. Relaxation aspectsof the liquid—glass transition. Uspekhi FizicheskihNauk. 2019;189(2): 113–133. DOI: https://doi.org/10.3367/ufnr.2018.04.0383192. Tsydypov Sh. B., Parfenov A. N., Sanditov D. S.,Agrafonov Yu. V., Nesterov A. S. 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Glass-forming ability is one of the most desired properties of organic compounds dedicated to optoelectronic applications. Therefore, finding general structure–property relationships and other rules governing vitrification and related near-glass-transition phenomena is a burning issue for numerous compound families, such as Schiff bases. Hence, we employ differential scanning calorimetry, broadband dielectric spectroscopy, X-ray diffraction and quantum density functional theory calculations to investigate near-glass-transition phenomena, as well as ambient- and high-pressure molecular dynamics for two structurally related Schiff bases belonging to the family of glycine imino esters. Firstly, the surprising great stability of the supercooled liquid phase is shown for these compounds, also under high-pressure conditions. Secondly, atypical self-organization via bifurcated hydrogen bonds into lasting centrosymmetric dimers is proven. Finally, by comparing the obtained results with the previous report, some general rules that govern ambient- and high-pressure molecular dynamics and near-glass transition phenomena are derived for the family of glycine imino esters. Particularly, we derive a mathematical formula to predict and tune their glass transition temperature (Tg) and its pressure coefficient (dTg/dp). We also show that, surprisingly, despite the presence of intra- and intermolecular hydrogen bonds, van der Waals and dipole–dipole interactions are the main forces governing molecular dynamics and dielectric properties of glycine imino esters.

In this thesis I present studies of a number of quantum many-body Bose systems via Quantum Monte Carlo methods. We investigated the dynamic structure factor of a hard-sphere Bose system simulated at T=0 at different densities, from the dilute to the strongly interacting regimes. By increasing the density we observed the spectrum evolves from the weakly interacting Bogoliubov to a phonon-maxon-roton dispersion, but also the emergence of a broad multi-quasiparticle component. For a system with sphere radius and density corresponding to superfluid 4He at equilibrium, we found good agreement with the spectrum in the roton region. In another work, a liquid of distinguishable 4He atoms near freezing at T=1 K was studied to compute the equation of state and static density response function. The results of this study have been used to improve the description of the superfluid-to-solid transition within the Density Functional Theory. Measurements of crystallization kinetics in supercooled liquid p-H2--o-D2 mixtures showed a slowdown with respect to the pure counterparts. In order to contribute to the interpretation of these results we simulated these metastable mixtures. We found differences in the quantum delocalization of the two isotopic molecules, which result in different effective sizes. We characterized also the differences in the local order around the molecules of each species. These results revealed that the observed slowdown is due to purely quantum effects. Finally, in a QMC study of ion Ar+ doped 4He nanodroplets at T=1 K, we computed density profiles, energies, and investigated local order around the Ar+ ion. We found stable solid structures around the ion composed of three solvation shells having the shape of platonic solids: an icosahedron, a dodecahedron, and, again, an icosahedron, with 12, 20, and 12 4He atoms, going from the inner to the outer shell respectively. These results confirmed the interpretation of experimental measurements of the abundances of Ar+@4He nanodroplets.