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Shaped ultrafast laser pulses were used to study and control the ionization dynamics of electronically excited pyrazine in a pump and probe experiment. For pump pulses created without feedback from the product signal, the ion growth curve (the parent ion signal as a function of pump/probe delay) was described quantitatively by the classical rate equations for internal conversion of the S2 and S1 states. Very different, non-classical behavior was observed when a genetic algorithm (GA) employing phase-only modulationwas used to minimize the ion signal at some pre-determined target time, T. Two qualitatively different control mechanisms were identified for early (T < 1.5 ps) and late (T > 1.5 ps) target times. In the former case, the ion signalwas largely suppressed for t < T,while for t » T, the ion signal produced by the GA-optimized pulse and a transform limited (TL) pulse coalesced. In contrast, for T > 1.5 ps, the ion growth curve followed the classical rate equations for t < T, while for t » T, the quantum yield for the GA-optimized pulse was much smaller than for a TL pulse. We interpret the first type of behavior as an indication that the wave packet produced by the pump laser is localized in a region of the S2 potential energy surface where the vertical ionization energy exceeds the probe photon energy, whereas the second type of behavior may be described by a reduced absorption cross section for S0 → S2 followed by incoherent decay of the excited molecules. Amplitude modulation observed in the spectrum of the shaped pulse may have contributed to the control mechanism, although this possibility is mitigated by the very small focal volume of the probe laser. [ABSTRACT FROM AUTHOR]

Pairs of 80 fs, 800 nm laser pulses were used to ablate Si, Cu, and CaF2 in air. The spectrally resolved plasma emission was measured as a function of laser fluence and pulse delay. After an initial dip, the fluorescence was found to increase monotonically with pulse delay, reaching a plateau after some tens of picoseconds, depending on the material and fluence. The enhancement ratio (defined as the ratio of the fluorescence produced by the pulse pair to that produced by a single pulse of the same total fluence) reaches a maximum value of 6 and 11 at a fluence of ∼6 J/cm2 for Si and Cu, respectively, and declines to a value below 2 at higher fluences. In contrast, the enhancement for CaF2 increases slowly from zero near threshold to a broad maximum value of 2 near 50 J/cm2. Using reflectivity and atomic force microscopy measurements as diagnostics, we interpret the Si and Cu behavior in terms of a two phase mechanism, in which the first pulse melts the surface of the crystal and the second pulse ablates the resulting liquid film. A qualitatively different mechanism initiated by multiphoton absorption is involved in CaF2 ablation. [ABSTRACT FROM AUTHOR]