In article number 2008109, Marius Buerkle, Satoshi Kaneko, Tomoaki Nishino, and co-workers induce the water-splitting reaction under visible light utilizing a copper-based single-molecule junction. A product (hydrogen) and a reactant (water-molecule) are distinguished by the single-molecule measurements techniques based on conductance measurement, inelastic electron tunneling spectroscopy, and the first-principles calculations.