The compounds that undergo photochromic reaction in the crystalline-state are rare and their reaction dynamics are not well characterized as a result of the low degree of interconversion ratios and/or instability of the photo-generated isomers in the solid phase. We have recently found that a rhodium Binuclear complex [ (RhCp
*)
2 (μ-CH
2)
2 (μ-O
2SSO
2) ] (Cp
*=η
5-C
5Me
5) having a photo-responsive dithionite group (μ-O
2SSO
2), undergoes an essentially 100% reversible crystalline-state photochromism upon interconversion to [ (RhCp
*)
2 (μ-CH
2)
2 (μ-O
2SOSO) ] . Taking an advantage of this unique full reversibility, we have investigated the dynamics of the system by using stepwise single crystal diffraction and variable-temperature solid-state NMR technique. The stereospecifc oxygen-atom rearrangement process of the dithionite ligand and reorientational motion of the Cp
* ligands, which are coupled to the photochromism, are presented.
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