Intervention mechanism of amphiphilic natural sweeteners on starch chain dynamic behavior: Computational and experimental insights.

Amphiphilic natural sweeteners (i.e. steviol glycosides (STE) and glycyrrhizic acid (GA)) have been adopted to improve the quality of various starchy products, which can fundamentally be characterized as the intervention of the former in the chain dynamic behavior of the latter. However, these phenomena and related mechanisms still lack systematic insights. Herein, dual-temperature molecular dynamic simulations combined with experimental analysis were used to tandemly investigate the intervention of sweeteners in six types of chain dynamic behaviors that are strongly correlated with starch properties, including unwinding, movement, long/short-term reassociation, rearrangement, and depolymerization. The results show that STE and GA both promoted the chain unwinding and movement, and also retarded the chain short/long-term reassociation and rearrangement. Besides, GA exhibited a greater role than STE in facilitating chain unwinding and movement. Peculiarly, GA (0 %-40 % w/w) collaborated with starch to form a new microstructure, especially at high content (≥ 20 % w/w), which endowed starch with exceptionally high hardness (15.50 gf→189.36 gf) and hardening rate (2.72 gf/d→17.76 gf/d), and also placed a physical barrier to retard starch depolymerization (slowly digestible starch: 11.26 %→20.62 %). This work contributes data and theoretical support for the development of starch/amphiphilic natural sweetener composite matrices.