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Photoswitchable diarylethenes (DAEs), over years of intense fundamental and applied research, have been established among the most commonly chosen molecular photoswitches, often employed as controlling units in molecular devices and smart materials. At the same time, providing reliable explanation for their photophysical behavior, especially the mechanism of the photo-cycloreversion transformation, turned out to be a highly challenging task. Herein, we investigate this mechanism in detail by means of multireference semi-empirical quantum
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