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Single molecules trapped in the solid state at liquid helium temperatures arepromising quantum emitters for the development of quantum technologies owing totheir remarkable photostability and their lifetime-limited optical coherencetime of the order of 10 ns. The coherent preparation of their electronic staterequires resonant excitation with a Rabi period much shorter than their opticalcoherence time. Sculpting the optical excitation with sharp edges and a highon-off intensity ratio ($\sim 3\times 10^5$) from a single-frequency laserbeam, we demonstrate sub-nanosecond drive of a single dibenzanthanthrenemolecule embedded in a naphthalene matrix at 3.2$^\circ$K, over more than 17Rabi periods. With pulses tailored for a half-Rabi period, the electronicexcited state is prepared with fidelity as high as 0.97. Using single-moleculeRamsey spectroscopy, we prove up to 5$^\circ$K that the optical coherencelifetime remains at its fundamental upper limit set by twice the excited-statelifetime, making single molecules suitable for quantum bit manipulations understandard cryogen-free cooling technologies.

Sub-nanosecond coherent optical manipulation of a single aromatic molecule at cryogenic temperature