Abstract A new class of ultrafast light-driven molecular switch has been designed and synthesized. The reaction of 1-substituted 2-methylidene-3, 3-dimethyl-2, 3-dihydro-1H- indoles with 2-chloromethyl-4-nitrophenol afforded 1′, 3, 3′, 4-tetrahydrospiro [chromene- 2, 2′-indoles], following a basic workup. The spectroscopic properties and nanosecond- resolved photoinduced dynamics of five compounds in the 1′, 3, 3′, 4-tetrahydrospiro [ ...