摘要： Molecular machines were attractive for scientists due to their excellent dynamical properties and potential applications. Inspired by the feature of molecular machine, we designed an ideal unscrewing process of double-chain sexipyridine complex with four conformations and explored the variation of stability and optical properties. As a result, we found the double helices where the fragments bound by only weak π-π interaction had poor stability. Thus the conformation with stronger π-π interaction was more stable than others. But this could be changed by adding alkali metals, and different alkali metal atoms such as Li and Na could control the stability order because of their different atomic radii. For Li-doped molecules, Li-1 with tightly coiled strands was the most stable conformation. While for Na-doped molecules, Na-4 with unscrewed fragments was the most stable one. This mainly resulted from the intra-molecular interaction potential energy especially the interaction between metal and ligand. At the same time, the charge distribution showed corresponding variation. In the aspect of optical properties, the unscrewing process was followed by the variation of absorption intensity at about 500 nm in the UV–Vis absorption spectra because of the conformation change. Meanwhile, the first-order static hyperpolarizability (βtot) showed zigzag variation due to the change of frontier molecular orbital energy gap in the unscrewing process.