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Photomechanical switches are light sensitive molecules capable of transducing the energy of a photon into mechanical work via photodynamics. In this Letter, we present the first atomistic investigation of the photodynamics of a novel class of photochromes called donor-acceptor Stenhouse adducts (DASA) using state-of-the-art ab initio multiple spawning interfaced with state-averaged complete active-space self-consistent field theory. Understanding the Z/E photoisomerization mechanism in DASAs at the molecular level is crucial in designing
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