Control over molecular nanostructure is of the utmost importance in bottom-up strategies to create functionalized surfaces for electronic devices and advanced materials. In this context, the study of two-dimensional self-assembled structures consisting of organic molecules on surfaces using scanning tunneling microscopy (STM) has been the subject of intensive research. The formation of stimuli-responsive assemblies, especially photoresponsive ones, on surfaces is attracting interest. Meanwhile, assemblies formed at the liquid/solid interface have been extensively studied using STM from a supramolecular chemistry perspective in order to understand the assembly process of the molecules from the solution phase to the substrate interface. In this review, an overview of advances in photoresponsive supramolecular self-assemblies formed at the liquid/solid interface is given. Recent progress in the analysis of the adsorption process using the nucleation–elongation model of two-dimensional self-assembly will be featured and discussed in the context of photochemical control of the assembly.

控制分子纳米结构在自下而上的策略中至关重要，以创建用于电子设备和先进材料的功能化表面。在此背景下，使用扫描隧道显微镜（STM）研究由表面上的有机分子组成的二维自组装结构已成为深入研究的主题。在表面上形成刺激响应组件，尤其是光响应组件，引起了人们的兴趣。同时，已从超分子化学的角度使用STM对在液/固界面处形成的组装体进行了广泛研究，以了解分子从溶液相到底物界面的组装过程。在这篇评论中，概述了在液体/固体界面形成的光响应性超分子自组装的进展。在使用光化学控制组件的背景下，将对使用二维自组装的成核-伸长模型分析吸附过程的最新进展进行专题介绍和讨论。