Correlated Fluctuations of Structural Indicators Close to the Liquid–Liquid Transition in Supercooled Water

The Journal of Physical Chemistry B, Год журнала: 2022, Номер 127(1), С. 378 - 386

Опубликована: Дек. 20, 2022

Multiple numerical studies have unambiguously shown the existence of a liquid-liquid critical point in supercooled states for different models water, and various structural indicators been put forward to describe transformation associated with this phase transition. Here we analyze simulations near-critical water compare behavior several such density fluctuations. We show that close most are strongly correlated density, some them even display identical distributions These probe exact same free energy landscape, therefore providing thermodynamic description which is provided by order parameter. This implies point, there tight coupling between many, only apparently distinct, degrees freedom.

Язык: Английский

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A Unified Description of the Liquid Structure, Static and Dynamic Anomalies, and Criticality of TIP4P/2005 Water by a Hierarchical Two-State Model

The Journal of Physical Chemistry B, Год журнала: 2023, Номер 127(15), С. 3452 - 3462

Опубликована: Апрель 12, 2023

Water has anomalous thermodynamic and kinetic properties distinct from ordinary liquids. The famous examples are the density maximum at 4 °C viscosity decrease upon pressurization. presence of second critical point been considered to be responsible for these anomalies since its discovery in ST2 water. Recently, existence confirmed firmly TIP4P/2005, which is one most successful classical models water, by Debenedetti et al. [Debenedetti Science 2020, 369, 289]. Here, we study water structure dynamic quantities a wide temperature (T)-pressure (P) range, including vicinity point, extensive molecular dynamics simulation this model. We reveal that hierarchical two-state model with cooperative formation tetrahedral structures via hydrogen bonding can describe T, P-dependences structure, anomalies, criticality TIP4P/2005 unified manner. shows very similar behaviors real all aspects, suggesting possible Our physical description based on two order parameters, fraction locally favored structures, indicates latter relevant parameter supported analysis fluctuations. different nature arrangements, conserved nonconserved, may key unambiguously identifying parameter.

Язык: Английский

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Measuring Entanglement in Physical Networks

Physical Review Letters, Год журнала: 2024, Номер 133(7)

Опубликована: Авг. 13, 2024

The links of a physical network cannot cross, which often forces the layout into nonoptimal entangled states. Here we define fabric as two-dimensional projection and propose average crossing number measure entanglement. We analytically derive dependence on density, link length, degree heterogeneity, community structure show that predictions accurately estimate entanglement both models real networks.

Язык: Английский

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Hierarchy of topological transitions in a network liquid

Proceedings of the National Academy of Sciences, Год журнала: 2024, Номер 121(36)

Опубликована: Авг. 29, 2024

The representation of complex systems as networks has become a critical tool across many fields science. In the context physical networks, such biological neural vascular or network liquids where nodes and edges occupy volume in three-dimensional space, question how they densely packed is special importance. Here, we investigate model liquid, which known to densify via two successive liquid–liquid phase transitions (LLPTs). We elucidate importance rings—cyclic paths formed by bonded particles networks—and their spatial disposition understanding structural changes that underpin increase density LLPTs. Our analyses demonstrate densification these primarily driven formation linked rings, LLPTs correspond hierarchy topological rings form fundamental building blocks. envisage entanglement emerge general mechanism for densification, with wide implications embedding especially confined spaces.

Язык: Английский

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Identification of local structures in water from supercooled to ambient conditions

The Journal of Chemical Physics, Год журнала: 2024, Номер 160(9)

Опубликована: Март 4, 2024

Studies of water thermodynamics have long been tied to the identification two distinct families local structures, whose competition could explain origin many thermodynamic anomalies and hypothesized liquid–liquid critical point in water. Despite successes insights gained, structural indicators proposed throughout years were not able unequivocally identify these over a wide range conditions. We show that recently introduced indicator, Ψ, which exploits information on hydrogen bond network connectivity, can reliably environments conditions (188–300 K 0–13 kbar) close point, spatial correlations density fluctuations are identical those Ψ indicator. Our results strongly support idea properties arise from between identifiable environments.

Язык: Английский

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Graph Theoretical Description of Phase Transitions in Complex Multiscale Phases with Supramolecular Assemblies

Advanced Science, Год журнала: 2024, Номер 11(33)

Опубликована: Июль 1, 2024

Phase transitions are typically quantified using order parameters, such as crystal lattice distances and radial distribution functions, which can identify subtle changes in crystalline materials or high-contrast phases with large structural differences. However, the identification of high complexity, multiscale organization complex patterns during fluctuations preceding phase transitions, essential for understanding system pathways between phases, is challenging those traditional analyses. Here, it shown that two model systems- thermotropic liquid crystals a lyotropic water/surfactant mixtures-graph theoretical (GT) descriptors successfully combining molecular nanoscale levels hard to characterize methodologies. Furthermore, GT also reveal different phases. Specifically, centrality parameters node-based fractal dimension quantify behavior capturing fluctuation-induced breakup aggregates their long-range cooperative interactions. parameterization be generalized wide range chemical systems instrumental growth mechanisms nanostructures.

Язык: Английский

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Complexity of confined water vitrification and its glass transition temperature

Proceedings of the National Academy of Sciences, Год журнала: 2024, Номер 121(41)

Опубликована: Окт. 2, 2024

The ability of vitrification when crossing the glass transition temperature (T g ) confined and bulk water is crucial for myriad phenomena in diverse fields, ranging from cryopreservation organs food to development cryoenzymatic reactions, frost damage buildings, atmospheric water. However, determining water’s T remains a major challenge. Here, we elucidate by analyzing calorimetric behavior nano-confined across various pore topologies (diameters: 0.3 2.5 nm). Our approach involves subjecting annealing protocols identify time evolution nonequilibrium kinetics. Furthermore, complement this with dynamics water, as seen broadband dielectric spectroscopy linear measurements, including fast scanning technique. This study demonstrated that undergoes range 170 200 K, depending on confinement size interaction walls. Moreover, also show thermal event observed at ~136 K must be interpreted an prepeak, referred “shadow transition.” Calorimetric measurements allow detection specific heat step above which insensitive and, thereby, true thermodynamic transition. Finally, connecting our results behavior, offer comprehensive understanding potential implications numerous applications.

Язык: Английский

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Kinetoplast DNA: a polymer physicist’s topological Olympic dream

Nucleic Acids Research, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 21, 2024

All life forms are miraculous, but some more inexplicable than others. Trypanosomes by far one of the most puzzling organisms on Earth: their mitochondrial genome, also called kinetoplast DNA (kDNA) an Olympic-ring-like network interlinked circles, challenging conventional paradigms in both biology and physics. In this review, I will discuss kDNA from astonished perspective a polymer physicist tell story how single sub-cellular structure blood-dwelling parasite is inspiring generations chemists physicists to create new catenated materials.

Язык: Английский

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TIP 4 P 2005 Ice : Simulating water with two molecular states

The Journal of Chemical Physics, Год журнала: 2025, Номер 162(1)

Опубликована: Янв. 7, 2025

Rigid, non-polarizable water models are very efficient from a computational point of view, and some them have great ability in predicting experimental properties. There is, however, little room for improvement simulating with this strategy, whose main shortcoming is that molecules do not change their interaction parameters response to the local molecular landscape. In work, we propose novel modeling strategy involves using two rigid as states can adopt depending on environment. During simulation, dynamically transition one state another order parameter quantifies structural feature. particular, belonging low- high-tetrahedral environments represented TIP4P/2005 TIP4P/Ice models, respectively. way, between strengthened when they acquire tetrahedral coordination, which be viewed an effective way introducing polarization effects. We call resulting model TIP4P2005Ice show it outperforms either build it. This multi-state only slows down simulations by factor 1.5 compared standard holds promise improving aqueous solutions.

Язык: Английский

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Effects of gravity on supersolid order in bubble-trapped bosons

Physical review. B./Physical review. B, Год журнала: 2025, Номер 111(2)

Опубликована: Янв. 27, 2025

Язык: Английский

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