Marazzi, MarcoGarcia-Iriepa, CristinaBenitez-Martin, CarlosNajera, FranciscoMonari, AntonioSampedro, Diego2025-01-072025-01-072021-12-01https://hdl.handle.net/10668/25311Nonlinear optical techniques as two-photon absorption (TPA) have raised relevant interest within the last years due to the capability to excite chromophores with photons of wavelength equal to only half of the corresponding one-photon absorption energy. At the same time, its probability being proportional to the square of the light source intensity, it allows a better spatial control of the light-induced phenomenon. Although a consistent number of experimental studies focus on increasing the TPA cross section, very few of them are devoted to the study of photochemical phenomena induced by TPA. Here, we show a design strategy to find suitable E/Z photoswitches that can be activated by TPA. A theoretical approach is followed to predict the TPA cross sections related to different excited states of various photoswitches' families, finally concluding that protonated Schiff-bases (retinal)-like photoswitches outperform compared to the others. The donor-acceptor substitution effect is therefore rationalized for the successful TPA activatable photoswitch, in order to maximize its properties, finally also forecasting a possible application in optogenetics. Some experimental measurements are also carried out to support our conclusions.enAttribution 4.0 Internationalhttp://creativecommons.org/licenses/by/4.0/EZ photoswitchesphotoisomerizationtwo-photon absorptionAzobenzene photoswitchesOne-photonPhotochemical characterizationPhotoisomerization dynamicsBenzylidene-oxazolonesCaged compoundsQuantum yieldLightSwitchesChromophoresresearch article34885961open access10.3390/molecules262373791420-3049https://www.mdpi.com/1420-3049/26/23/7379/pdf?version=1638693823734584600001