Abstract
We demonstrate control of the carrier-envelope phase of ultrashort periodic waveforms that are synthesized from a Raman-generated optical frequency comb. We generated the comb by adiabatically driving a molecular vibrational coherence with a beam at a fundamental frequency plus its second harmonic. Heterodyne measurements show that full interpulse phase locking of the comb components is realized. The results set the stage for the synthesis of periodic arbitrary waveforms in the femtosecond and subfemtosecond regimes with full control. © 2009 The American Physical Society.