This feature article covers the recent applications of metal‐organic framework nanoparticles (MOF NPs) in photodynamic therapy (PDT) of cancer. It aims at giving the reader an overview about these two current research fields, i.e., MOF and PDT, and at highlighting the potential synergistic effect that could result from their association. After describing the general photophysics and photochemistry that underlie PDT, the relationship between photosensitizer (PS) properties and PDT requirements is discussed throughout the PSs historical development. This development reveals the advantages of using nanotechnology platforms for the creation of the ideal PS and leads us to define the fourth generation of PSs, which includes NPs built from the PS itself as porphysomes or PS‐based MOF NPs. Especially, the precise spatial control over the PS assembly into well‐defined MOF NPs, which keeps the PS in its monomeric form and prevents PS self‐quenching, appears as a notable feature to solve PS solubility and aggregation issues and therefore improves the PDT efficiency. Finally, we discuss the future perspectives of MOF NPs in PDT and shed light on how promising these nanomaterials are.

Two-color sum-frequency generation spectroscopy (2C-SFG) is used to probe the molecular and electronic properties of an adsorbed layer of the green fluorescent protein mutant 2 (GFPmut2) on a platinum (111) substrate. First, the spectroscopic measurements, performed under different polarization combinations, and atomic force microscopy (AFM) show that the GFPmut2 proteins form a fairly ordered monolayer on the platinum surface. Next, the nonlinear spectroscopic data provide evidence of particular coupling phenomena between the GFPmut2 vibrational and electronic properties. This is revealed by the occurrence of two doubly resonant sum-frequency generation processes for molecules having both their Raman and infrared transition moments in a direction perpendicular to the sample plane. Finally, our 2C-SFG analysis reveals two electronic transitions corresponding to the absorption and fluorescence energy levels which are related to two different GFPmut2 conformations: the B (anionic) and I forms, respectively. Their observation and wavelength positions attest the keeping of the GFPmut2 electronic properties upon adsorption on the metallic surface.

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