Controlling the triplet states and their application in external stimuli-responsive triplet-triplet-annihilation photon upconversion: from the perspective of excited state photochemistry.

The property of organic light-responsive materials is determined by their electronic excited states to a large extent, for instance, the radiative decay rate constants, redox potentials, and lifetimes. Tuning the excited state properties with external stimuli will lead to versatile functional materials; a representative example is the fluorescence molecular probes, in which the singlet excited states are controlled by the external stimuli, i.e., by interaction with the analytes. In comparison, controlling the triplet excited state with external stimuli has been rarely reported, although it is also crucial for the development of novel materials for targeted photodynamic therapy (PDT) reagents and phosphorescent molecular probes. The reported results show that the principles used in singlet excited state tuning are unable to be simply applied to the triplet excited state. In this review article, we summarized the recent results on controlling the triplet excited states by the external stimuli (chemical or light), and the application of the triplet state tuning in the chemical/light controllable triplet-triplet-annihilation upconversion (TTA UC). We discussed the methods for the control of the triplet states, as well as singlet excited state, for the purpose of controlling the TTA UC. Both successful and unsuccessful methods are discussed. This information is helpful for understanding the photophysical processes in which the triplet excited state is involved, and the development of novel external stimuli-responsive triplet photosensitizers.