Predicting Spontaneous Orientational Self-Assembly: In Silico Design of Materials with Quantum Mechanically Derived Force Fields,The Journal of Physical Chemistry Letters

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Predicting Spontaneous Orientational Self-Assembly: In Silico Design of Materials with Quantum Mechanically Derived Force Fields
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2021-12-30 , DOI: 10.1021/acs.jpclett.1c03517
Giacomo Prampolini ₁ , Leandro Greff da Silveira ₂ , J G Vilhena ₃ , Paolo Roberto Livotto ₂

Affiliation

De novo design of self-assembled materials hinges upon our ability to relate macroscopic properties to individual building blocks, thus characterizing in such supramolecular architectures a wide range of observables at varied time/length scales. This work demonstrates that quantum mechanical derived force fields (QMD-FFs) do satisfy this requisite and, most importantly, do so in a predictive manner. To this end, a specific FF, built solely based on the knowledge of the target molecular structure, is employed to reproduce the spontaneous transition to an ordered liquid crystal phase. The simulations deliver a multiscale portrait of such self-assembly processes, where conformational changes within the individual building blocks are intertwined with a 200 ns ensemble reorganization. The extensive characterization provided not only is in quantitative agreement with the experiment but also connects the time/length scales at which it was performed. Realizing QMD-FF predictive power and unmatched accuracy stands as an important leap forward for the bottom-up design of advanced supramolecular materials.

中文翻译：

预测自发定向自组装：具有量子力学衍生力场的材料的计算机设计

从头自组装材料的设计取决于我们将宏观性质与单个构建块联系起来的能力，从而在这种超分子结构中表征在不同时间/长度尺度上的广泛可观察性。这项工作表明，量子力学派生力场 (QMD-FFs) 确实满足了这一要求，最重要的是，它以预测的方式满足了这一要求。为此，仅基于目标分子结构的知识构建的特定 FF 用于再现自发转变为有序液晶相。模拟提供了这种自组装过程的多尺度画像，其中单个构建块内的构象变化与 200 ns 的整体重组交织在一起。所提供的广泛表征不仅与实验在定量上一致，而且还连接了进行实验的时间/长度尺度。实现 QMD-FF 的预测能力和无与伦比的准确性是先进超分子材料自下而上设计的重要飞跃。

更新日期：2022-01-13

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