Demonstration of a HeNe/CH4-based optical molecular clock

We implement a simple optical clock based on the F2(2) P(7), v3] optical transition in methane. A single femtosecond laser's frequency comb undergoes difference frequency generation to provide an IR comb at 3.39 microm with a null carrier-envelope offset. This IR comb provides a phase-coherent link between the 88-THz optical reference and the rf repetition rate. Comparison of the repetition rate signal with a second femtosecond comb stabilized to molecular iodine shows an instability of 1.2 x 10(-13) at 1 s, limited by microwave detection of the repetition rates. The single-sideband phase noise of the microwave signal, normalized to a carrier frequency of 1 GHz, is below -93 dBc/Hz at 1-Hz offset.