Abstract
Carrier-envelope phase (CEP) dependence of high-order harmonic generation (HHG) from H2+ in a multi-cycle laser pulse is investigated by solving the non-Born-Oppenheimer time-dependent Schrödinger equation (TDSE). It is found that high harmonics in the plateau exhibit counterintuitive frequency modulation (FM) as the CEP of the multi-cycle laser varies. Based on the classical electron trajectories and time-frequency analysis, this multi-cycle CEP-dependent FM is demonstrated to result from the interference of half-cycle HHG radiations, which is modulated by laser-driven nuclear motion. The mechanism of the CEP-dependent FM is further confirmed by simulations based on a simple algorithm in the time domain, which satisfactorily reproduces the TDSE results. The CEP-dependent FM encodes rich information on the correlated electron and nuclear dynamics, which paves the way for probing nuclear motion with attosecond resolution.
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