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Synthetic molecular systems undergoing structure and property changes as a response to external stimuli offer a series of relevant functions. Their direct use in solution, immobilized at surfaces, or integrated into adequate matrices, allow for the elaboration of nano-carriers, molecular electronic memory circuits, adaptive systems, artificial muscles, or healable materials, among others. Reversible systems are commonly generated by utilizing molecular switches as responsive bi-stable molecules. Of particular interest are switches controlled by non-invasive triggers, especially light, which can display high spatial and temporal resolution. Photoswitches were used to change properties, such as conductance and basicity, based on light-induced alteration of the molecular geometry, that is, their dimensions and shape. In nature, light-induced geometrical modifications of molecular systems lead to primary biological functions, such as the visual perception in vertebrates, or proton pumping in some bacteria, two examples that nicely illustrate the potential of photo-inducing structural modifications in organic systems.