Title: Mean-field models for the chemical fueling of transient soft matter states Show Chinese title

Title: 瞬时软物质状态的化学供能的平均场模型

Abstract: The chemical fueling of transient states (CFTS) is a powerful process to control the nonequilibrium structuring and the homeostatic function of adaptive soft matter systems. Here, we introduce a mean-field model of CFTS based on the activation of metastable equilibrium states in a tilted Landau bistable energy landscape along a coarse-grained reaction coordinate (or order parameter) triggered by a nonmonotonic two-step chemical fueling reaction. Evaluation of the model in the quasi-static (QS) limit - valid for fast system relaxation - allows us to extract useful analytical laws for the critical activation concentration and duration of the transient states in dependence of physical parameters, such as rate constants, fuel concentrations, and the system's distance to its equilibrium transition point. We apply our model in the QS limit to recent experiments of CFTS of collapsing responsive microgels and find a very good performance with only a few global and physically interpretable fitting parameters, which can be employed for programmable material design. Moreover, our model framework also allows a thermodynamic analysis of the energy and performed work in the system. Finally, we go beyond the QS limit, where the system's response is slow and retarded versus the chemical reaction, using an overdamped Smoluchowski approach. The latter demonstrates how internal system time scales can be used to tune the time-dependent behavior and programmed delay of the transient states in full nonequilibrium. Show Chinese abstract

Abstract: 瞬态状态的化学供能（CFTS）是一个强大的过程，用于控制适应性软物质系统的非平衡结构和稳态功能。 在这里，我们介绍了一个基于倾斜Landau双稳态能量景观中亚稳平衡态激活的CFTS平均场模型，该模型由一个非单调两步化学供能反应沿粗粒度反应坐标（或序参数）触发。 在准静态（QS）极限下评估该模型——适用于系统快速弛豫的情况——使我们能够提取关于临界激活浓度和瞬态状态持续时间的有用解析定律，这些定律依赖于物理参数，如速率常数、燃料浓度以及系统与其平衡转变点的距离。 我们将该模型应用于QS极限下的最近CFTS实验，研究坍塌响应微凝胶，并发现其性能非常好，仅需几个全局且具有物理解释的拟合参数，这些参数可用于可编程材料设计。 此外，我们的模型框架还允许对系统中的能量和所做的功进行热力学分析。 最后，我们超越了QS极限，其中系统响应相对于化学反应较慢且滞后，使用过阻尼Smoluchowski方法。 后者展示了如何利用系统内部的时间尺度来调节瞬态状态的时间依赖行为和程序化延迟，在完全非平衡状态下实现。