Spider silk is a remarkable biomaterial with exceptional stiffness, strength, and toughness stemming from a unique microstructure. While recent studies show that silk fibers exhibit plasticity, hysteresis, and recovery under cyclic loading, the underlying microstructural mechanisms are not yet fully understood. In this work, we propose a mechanism explaining the loading-unloading-relaxation response through microstructural evolution: initial loading distorts intermolecular bonds, resulting in a linear elastic regime. Upon reaching the yield stress, these bonds dissociate and the external load is transferred to the polypeptide chains, which deform entropically to allow large deformations. Unloading is driven by entropic shortening until a traction free state with residual stretch is achieved. Subsequently, the fiber recovers as chains reorganize and bonds reform, locking the microstructure into a new stable equilibrium that increases stiffness in subsequent cycles. Following these mechanisms, we develop a microscopically motivated, energy-based model that captures the macroscopic response of silk fibers under cyclic loading. The response is decoupled into two parallel networks: (1) an elasto-plastic network of inter- and intramolecular bonds governing the initial stiffness and yield stress, and (2) an elastic network of entropic chains that enable large deformations. The model is validated against experimental data from Argiope bruennichi dragline silk. The findings from this work are three-fold: (1) explaining the mechanisms that govern hysteresis and recovery and linking them to microstructural evolution; (2) quantifying the recovery process of the fiber, which restores and enhances mechanical properties; and (3) establishing a predictive foundation for engineering synthetic fibers with customized properties.
Olivé et al. (Wed,) studied this question.