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The first examples of single crystals exhibiting salient effects by different structure change mechanisms are reported. The crystals of newly prepared aryl(9-isocyanoanthracene)gold(I) complexes jump in response to two different external stimuli ultraviolet (UV) irradiation and cooling. The photosalient effect is triggered by photodimerization reaction of the anthracene moieties under photoirradiation. By contrast, the thermosalient effect is caused by anisotropic thermal contraction upon cooling without a chemical structure change. By

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