Waveform Synthesis of Attosecond Optical Pulses: A Common Route to Attosecond Pump-Probe Spectroscopy and Nanoscopy in Aqueous Solution

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When a molecule absorbs light, its electronic cloud reacts almost instantaneously followed by rovibrational nuclear dynamics on the femtosecond (fs=10-15s.) to picosecond (ps=10-12s.) timescale. In photosynthesis, for example, the absorption of ultraviolet light by chlorophyll molecules induces an electronic dipole oscillation, which has a period in the range of 1 fs, followed by its slower decay and energy redistribution to the nuclear degrees of freedom. Over the last decades, time-resolved spectroscopy showed how few-cycle femtosecond laser pulses can be used to steer nuclear wave packets and control the outcome of elementary reactions. The lack of shorter pulses, however, has left control of the electron wave packets on the sub-oscillation period timescale unexplored. Would it be possible to follow and, ultimately, more efficiently control reaction dynamics right from the earliest moments when electron dipole forces initiate nuclear motion?