Shine a light: a circular dichroism effect in the ±10 % regime on randomly oriented chiral molecules in the gas phase is demonstrated. The signal is derived from images of photoelectron angular distributions produced by resonance-enhanced multiphoton ionization and allows the enantiomers to be distinguished. To date, this effect could only be generated with a synchrotron source. The new tabletop laser-based approach will make this approach far more accessible.

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Ionization mechanisms in water irradiated with bandwidth-limited and temporally asymmetric femtosecond laser pulses are investigated via ultrafast spectral interferometry. By using a novel common-path interferometer with an enlarged temporal measurement window, we directly observe the dynamics of free-electron plasma generated by shaped pulses. We found that a temporally asymmetric pulse and its time-reversed counterpart address multiphoton and avalanche ionization mechanisms in a different fashion. Positive third-order dispersion shaped pulses produce a much higher free-electron density than negative ones at the same fluence, instantaneous frequency and focusing conditions. From the experimental data obtained after irradiation with bandwidth-limited and shaped pulses the multiphoton and avalanche coefficients were determined using a generic rate equation. We conclude that temporal tailored femtosecond pulses are suitable for manipulation of the initial steps in laser processing of high band gap materials.

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We investigate the temporal precision in the generation of ultrashort laser pulse pairs by pulse shaping techniques. To this end, we combine a femtosecond polarization pulse shaper with a polarizer and employ two linear spectral phase masks to mimic an ultrastable common-path interferometer. In an all-optical experiment we study the interference signal resulting from two temporally delayed pulses. Our results show a 2σ-precision of 300 zs = 300 × 10(-21) s in pulse-to-pulse delay. The standard deviation of the mean is 11 zs. The obtained precision corresponds to a variation of the arm's length in conventional delay stage based interferometers of 0.45 Å. We apply these precisely generated pulse pairs to a strong-field quantum control experiment. Coherent control of ultrafast electron dynamics via photon locking by temporal phase discontinuities on a few attosecond timescale is demonstrated.