Network approach towards understanding the crazing in glassy amorphous polymers

TL;DR

This study employs molecular dynamics and network theory to analyze the deformation mechanisms of crazing in glassy amorphous polymers, revealing the distinct roles of Van der Waals and entanglement networks during deformation stages.

Contribution

It introduces a novel network-based approach to understand crazing in polymers, linking molecular interactions to macroscopic deformation behavior.

Findings

Van der Waals network is crucial for craze initiation and growth.

Entanglement network weakens during hardening and failure stages.

Network measures correlate with stress-strain and void statistics.

Abstract

We have used molecular dynamics to simulate an amorphous glassy polymer with long chains to study deformation mechanism of crazing and associated void statistics. The Van der Waals interactions and the entanglements between chains constituting the polymer play a crucial role in crazing. Thus, we have reconstructed two underlying weighted networks, namely, the Van der Waals network and the Entanglement network from polymer configurations extracted from the molecular dynamics simulation. Subsequently, we have performed graph-theoretic analysis of the two reconstructed networks to reveal the role played by them in crazing of polymers. Our analysis captured various stages of crazing through specific trends in the network measures for Van der Waals networks and entanglement networks. To further corroborate the effectiveness of network analysis in unraveling the underlying physics of crazing in polymers, we have contrasted the trends in network measures for Van der Waals networks and entanglement networks in the light of stress-strain behaviour and voids statistics during deformation. We find that Van der Waals network plays a crucial role in craze initiation and growth. Although, the entanglement network was found to maintain its structure during craze initiation stage, it was found to progressively weaken and undergo dynamic changes during the hardening and failure stages of crazing phenomena. Our work demonstrates the utility of network theory in quantifying the underlying physics of polymer crazing and widens the scope of applications of network science to characterization of deformation mechanisms in diverse polymers.