Autonomous active, elastic filaments that interact with each other to achieve cooperation and synchrony underlie many critical functions in biology. The mechanisms underlying this collective response and the essential ingredients for stable synchronization remain a mystery. Inspired by how these biological entities integrate elasticity with molecular motor activity to generate sustained oscillations, a number of synthetic active filament systems have been developed that mimic oscillations of these biological active filaments. Here, we describe the collective dynamics and stable spatiotemporal patterns that emerge in such biomimetic multi-filament arrays, under conditions where steric interactions may impact or dominate the collective dynamics. To focus on the role of steric interactions, we study the system using Brownian dynamics, without considering long-ranged hydrodynamic interactions. The simulations treat each filament as a connected chain of self-propelling colloids. We demonstrate that short-range steric inter-filament interactions and filament roughness are sufficient - even in the absence of inter-filament hydrodynamic interactions - to generate a rich variety of collective spatiotemporal oscillatory, traveling and static patterns. We first analyze the collective dynamics of two- and three-filament clusters and identify parameter ranges in which steric interactions lead to synchronized oscillations and strongly occluded states. Generalizing these results to large one-dimensional arrays, we find rich emergent behaviors, including traveling metachronal waves, and modulated wavetrains that are controlled by the interplay between the array geometry, filament activity, and filament elasticity. Interestingly, the existence of metachronal waves is non-monotonic with respect to the inter-filament spacing. We also find that the degree of filament roughness significantly affects the dynamics - specifically, filament roughness generates a locking-mechanism that transforms traveling wave patterns into statically stuck and jammed configurations. Taken together, simulations suggest that short-ranged steric inter-filament interactions could combine with complementary hydrodynamic interactions to control the development and regulation of oscillatory collective patterns. Furthermore, roughness and steric interactions may be critical to the development of jammed spatially periodic states; a spatiotemporal feature not observed in purely hydrodynamically interacting systems.
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http://dx.doi.org/10.1039/d0sm01162b | DOI Listing |
Biochemistry
January 2025
Biomolecular Research Institute, Boise State University, 1910 University Drive, Boise, Idaho 83725, United States.
The amino-terminal domain of collagen α1(XI) plays a key role in controlling fibrillogenesis. However, the specific mechanisms through which various isoforms of collagen α1(XI) regulate this process are not fully understood. We measured the kinetics of collagen type I self-assembly in the presence of specific collagen α1(XI) isoforms.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Department of Chemistry and Biochemistry, University of California, San Diego, La Jolla, California 92093-0309, United States.
Controlling molecular actions on demand is a critical step toward developing single-molecule functional devices. Such control can be achieved by manipulating the interactions between individual molecules and their nanoscale environment. In this study, we demonstrate the conformational transition of a single pyrrolidine molecule adsorbed on a Cu(100) surface, driven by vibrational excitation through tunneling electrons using scanning tunneling microscopy.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
RIKEN: Rikagaku Kenkyujo, Center for Sustainable Resource Science, 2-1 Hirosawa, 351-0198, Wako, JAPAN.
Transition-metal-catalyzed selective and efficient activation of an inert C-H bond in an organic substrate is of importance for the development of streamlined synthetic methodologies. An attractive approach is the design of a metal catalyst capable of recognizing an organic substrate through noncovalent interactions to control reactivity and selectivity. We report here a spirobipyridine ligand that bears a hydroxy group that recognizes pyridine and quinoline substrates through hydrogen bonding, and in combination with an iridium catalyst enables site-selective C-H borylation.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China.
The comprehensive understanding of the effect of the chemical environment surrounding active sites on the pathway for the electrochemical carbon dioxide reduction reaction (eCORR) is essential for the development of advanced catalysts for large-scale applications. Based on a series of model catalysts engineered by the coordination of copper ions with various isomers of phenylenediamine [i.e.
View Article and Find Full Text PDFChemphyschem
January 2025
University of North Carolina, Research Computing Center, 211 Manning Drive, 27599-3420, Chapel Hill, UNITED STATES OF AMERICA.
Covalent bonding and noncovalent interactions are important chemical concepts and how to identify them has been of current interest in the literature. Within the framework of density functional theory (DFT), we recently proposed a few qualitative descriptors to categorize different types of interactions with Pauli energy and its derivatives. In this work, we expand the scope by including the quantities derived from energetic information, which were recently proposed and thoroughly investigated by us from the framework of information-theoretic approach (ITA) in DFT.
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