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Firstly, the nearly planar acyclic chalcone derivatives were inclined to undergo photo\u2010induced stereospecific [2+2] cycloaddition, which triggered the crystals to exhibit macroscopic motions of bending or cracking. In particular, the single\u2010crystal\u2010to\u2010single\u2010crystal transformation happened upon UV irradiation of the crystals, which was helpful for the understanding photomechanical effects. Cyclic 3,4\u2010dihydronaphthalene\u2010based chalcone analogues possess a more twisted conformation, and they tend to undergo <jats:italic>trans\u2010cis<\/jats:italic> isomerization. No photomechanical effect was observed for the crystals of the cyclic chalcone analogues due to the lower isomerization rate. The twist degree of chroman\u2010based molecules was in between of the first two, [2+2] cycloaddition and <jats:italic>trans\u2010cis<\/jats:italic> isomerization simultaneously took place in crystals. Photo\u2010induced bending and twisting were observed for the crystals of chroman\u2010based chalcone analogues. Therefore, the differences in molecular dihedral angles in \u03b1,\u03b2\u2010unsaturated ketones were responsible for their photochemical characters and in turn to tune the photomechanical effects. In this work, a bridge between the molecular structures and solid\u2010state photochemical reactions triggered photomechanical crystals is built.<\/jats:p>","DOI":"10.1002\/chem.202203178","type":"journal-article","created":{"date-parts":[[2022,11,7]],"date-time":"2022-11-07T22:29:38Z","timestamp":1667860178000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":16,"title":["Molecular Twisting Affects the Solid\u2010State Photochemical Reactions of Unsaturated Ketones and the Photomechanical Effects of Molecular Crystals"],"prefix":"10.1002","volume":"29","author":[{"given":"Yuan","family":"Yue","sequence":"first","affiliation":[{"name":"State Key Laboratory of Supramolecular Structure and Materials College of Chemistry Jilin University  Changchun 130021 P. R. 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