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We have used kinetic Monte Carlo simulations to study the kinetics ofunfolding of cross-linked polymer chains under mechanical loading. As the endsof a chain are pulled apart, the force transmitted by each crosslink increasesuntil it ruptures. The stochastic crosslink rupture process is assumed to begoverned by first order kinetics with a rate that depends exponentially on thetransmitted force. We have performed random searches to identify optimalcrosslink configurations whose unfolding requires a large applied force(measure of strength) and/or large dissipated energy (measure of toughness). Wefound that such optimal chains always involve cross-links arranged to formparallel strands. The location of those optimal strands generally depends onthe loading rate. Optimal chains with a small number of cross-links were foundto be almost as strong and tough as optimal chains with a large number ofcross-links. Furthermore, optimality of chains with a small number ofcross-links can be easily destroyed by adding cross-links at random. Thepresent findings are relevant for the interpretation of single molecule forceprobe spectroscopy studies of the mechanical unfolding of load-bearingproteins, whose native topology often involves parallel strand arrangementssimilar to the optimal configurations identified in the study

physical review. e, statistical, nonlinear and soft matter physics

Theoretical studies of the kinetics of mechanical unfolding of cross-linked polymer chains and their implications for single-molecule pulling experiments