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High-Density "Windowpane" Coordination Patterns of Water Clusters and Their NBO/NRT Characterization.

ABSTRACT: Cluster mixture models for liquid water at higher pressures suggest the need for water clusters of higher coordination and density than those commonly based on tetrahedral H-bonding motifs. We show here how proton-ordered water clusters of increased coordination and density can assemble from a starting cyclic tetramer or twisted bicyclic (Möbius-like) heptamer to form extended Aufbau sequences of stable two-, three-, and four-coordinate "windowpane" motifs. Such windowpane clusters exhibit sharply reduced (~90°) bond angles that differ appreciably from the tetrahedral angles of idealized crystalline ice I_h. Computed free energy and natural resonance theory (NRT) bond orders provide quantitative descriptors for the relative stabilities of clusters and strengths of individual coordinative linkages. The unity and consistency of NRT description is demonstrated to extend from familiar supra-integer bonds of the molecular regime to the near-zero bond orders of the weakest linkages in the present H-bond clusters. Our results serve to confirm that H-bonding exemplifies resonance-covalent (fractional) bonding in the sub-integer range and to further discount the dichotomous conceptions of "electrostatics" for intermolecular bonding vs. "covalency" for intramolecular bonding that still pervade much of freshman-level pedagogy and force-field methodology.

SUBMITTER: Weinhold F

PROVIDER: S-EPMC9268199 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:IntroductionElectrical contact mapping provides a detailed view of conduction patterns in the atria during atrial fibrillation (AF). Identification of repetitive wave front propagation mechanisms potentially initiating or sustaining AF might provide more insights into temporal and spatial distribution of candidate AF mechanism and identify targets for catheter ablation. We developed a novel tool based on recurrence plots to automatically identify and characterize repetitive conduction patterns in high-density contact mapping of AF.Materials and methodsRecurrence plots were constructed by first transforming atrial electrograms recorded by a multi-electrode array to activation-phase signals and then quantifying the degree of similarity between snapshots of the activation-phase in the electrode array. An AF cycle length dependent distance threshold was applied to discriminate between repetitive and non-repetitive snapshots. Intervals containing repetitive conduction patterns were detected in a recurrence plot as regions with a high recurrence rate. Intervals that contained similar repetitive patterns were then grouped into clusters. To demonstrate the ability to detect and quantify the incidence, duration and size of repetitive patterns, the tool was applied to left and right atrial recordings in a goat model of different duration of persistent AF [3 weeks AF (3 wkAF, n = 8) and 22 weeks AF (22 wkAF, n = 8)], using a 249-electrode mapping array (2.4 mm inter-electrode distance).ResultsRecurrence plots identified frequent recurrences of activation patterns in all recordings and indicated a strong correlation between recurrence plot threshold and AF cycle length. Prolonged AF duration was associated with shorter repetitive pattern duration [mean maximum duration 3 wkAF: 74 cycles, 95% confidence interval (54-94) vs. 22 wkAF: 41 cycles (21-62), p = 0.03], and smaller recurrent regions within repetitive patterns [3 wkAF 1.7 cm2 (1.0-2.3) vs. 22 wkAF 0.5 cm2 (0.0-1.2), p = 0.02]. Both breakthrough patterns and re-entry were identified as repetitive conduction patterns.ConclusionRecurrence plots provide a novel way to delineate high-density contact mapping of AF. Dominant repetitive conduction patterns were identified in a goat model of sustained AF. Application of the developed methodology using the new generation of multi-electrode catheters could identify additional targets for catheter ablation of AF.

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High-Density "Windowpane" Coordination Patterns of Water Clusters and Their NBO/NRT Characterization.

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