Theory for dynamic matter: designing mechanisms for dissipative nanomaterials

Jason R.马萨诸塞州波士顿大学的绿色得到了化学系化学理论、模型和计算方法项目的支持，以促进我们对化学如何控制活性材料的形式和功能的基本理解。 活性材料是被设计成具有一种或多种性质的材料，这些性质可以通过外部刺激（例如温度、光或化学反应）以受控方式显著改变。 在实验室中，化学反应用于组装，维持，调节和破坏由活性，反应分子制成的材料的结构。通过操纵化学反应，人们可以调整它们的性质。 这种材料具有许多潜在的应用，例如在药物递送和生物传感中。然而，这些材料的性质取决于结构形成的历史和细节。 因此，从组成分子构建块的性质预测产量和机械行为是一个挑战。绿色教授和同事们正在开发理论框架来克服这一挑战。他们的目标是提供洞察物质的动态能力，以找到稳定的替代路线，功能结构时，由化学能燃料。绿色教授还创建了开放科学计算笔记本，其中包含可访问的，计算上易处理的，实验相关的自组装模型。自组装作为一种合成复杂材料的简单技术，具有实际应用前景。分子组分组织成活性材料，当它们耗散能量时只能暂时维持结构。主要的挑战是理解材料性质的时间依赖性和改变反应条件的影响。该项目正在开发适当的理论框架，以了解非平衡力如何共同驱动结构形成并塑造组装路径的广阔空间。我们的目标是预测哪些途径是典型的，哪些是罕见的，在宏观尺度上从随机化学动力学，准确地模拟实验。这项研究有三大贡献：在活性材料的非平衡组装的建模和模拟方面取得进展，在识别组装模式和结构形成的因果机制的理论和实践方面取得进展，并收集随机热力学数据库，该奖项反映了NSF的法定使命，并被认为是值得通过使用基金会的知识价值和更广泛的影响审查标准。

Professor Jason R. Green of the University of Massachusetts Boston is supported by an award from the Chemical Theory, Models and Computational Methods Program in the Chemistry Division to advance our fundamental understanding of how chemistry controls the form and the function of active materials. Active materials are materials designed to have one or more properties that can be significantly changed in a controlled fashion by external stimuli such as temperature, light, or chemical reactions. In the laboratory, chemical reactions are used to assemble, sustain, regulate, and destroy the structure of materials made from active, responsive molecules. By manipulating the chemical reactions, one can tune their properties. Such materials have many potential applications, for example in drug delivery and biosensing. However, the properties of these materials depend on the history and the details of how the structure was formed. As a result, it is a challenge to predict the yield and mechanical behavior from the properties of the constituent molecular building blocks. Professor Green and coworkers are developing theoretical frameworks to overcome this challenge. Their goal is to provide insight into the dynamic ability of matter to find alternative routes to stable, functional structures when fueled by chemical energy. Professor Green is also creating open-science computational notebooks that contain accessible, computationally tractable, and experimentally-relevant models for self-assembly.Self-assembly has practical promise as a simple technique to synthesize complex materials. Molecular components organize into active materials that can only sustain structure transiently as they dissipate energy. The principal challenges are understanding the time dependence of material properties and the effect of changing reaction conditions. This project is developing appropriate theoretical frameworks for understanding how non-equilibrium forces collectively drive structure formation and sculpt the vast space of assembly pathways. The goal is to predict which pathways are typical and which are rare at the macroscopic scale from stochastic chemical-kinetics that accurately model experiments. This research is making three major contributions: advancing in the modeling and simulation of the nonequilibrium assembly of active materials, advancing in the theory and practice for identifying the assembly patterns and causal mechanisms of structure formation, and collecting the stochastic-thermodynamics for a database of self-assembly models at and evolving away from equilibrium.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.