Pairs of ultrafast laser pulses are used to ablate Si⟨111⟩. The fluorescence from Si atoms and ions was observed to increase by an order of magnitude as the delay between the pulses was increased. From the dependence of the fluorescence enhancement on the laser fluence and the pulse delay, it is deduced that the first pulse melts the surface and that the second pulse interacts more strongly with the liquid phase.
The mass spectra of a series of cycloketone molecules, cyclopentanone (CPO), cyclohexanone (CHO), cycloheptanone (CHPO), and cyclooctanone (COO) are measured in a 788 or 394 nm laser field with 90 fs pulse duration and the intensity ranging from 5 x 10(13) W/cm(2) to 2 x 10(14) W/cm(2). At 788 nm, a dominated parent ion peak and some weak peaks from the fragment ions C(n)H(m)+ are observed for CPO and CHO (a ratio P(+)/T(+), the parent ion yield to the total ion yield, is 81.6% and 52.6%, respectively). But the extensive fragment ion peaks are observed with the greatly reduced parent ion peak for CHPO (P(+)/T(+) = 5.5%) and that are even hard to be identified for COO. These observations are interpreted explicitly in the frame of the significant resonant effect of their cation photoabsorption on ionization and dissociation of these molecules. The present work also suggests that a nonadiabatic ionization occurs with a nuclear rearrangement due to the H movement in these molecules during the ionization in an intense femtosecond laser field.
Pairs of 80fs, 800nm 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 ∼6J∕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 50J∕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.
The ionization/dissociation mechanism of cyclopentanone has been experimentally investigated in molecular beam by irradiating with intense 394 and 788 nm laser fields with pulse duration of 90 fs. The range of laser intensities varied from 3 x 10(13) to 4 x 10(14) W/cm(2). For both wavelengths, the singly charged parent ion is observable while the doubly charged one cannot be found easily, although the fragmentation pattern supports its presence. Meanwhile, the extent of fragmentation at 788 nm is less than that in the 394 nm case. We quantitatively analyze the ionization processes of cyclopentanone in intense femtosecond laser by comparing the calculation results of ionization rate constants obtained from Ammosov-Delone-Krainov, Keldysh, and Keldysh-Faisal-Reiss (KFR) theories based on hydrogenlike atom model. We also compare the experimental and theoretical results; the generalized KFR theory is found to be useful in predicting the ionization yields of singly and doubly charged cyclopentanone ion. To interpret the dissociation patterns of the cyclopentanone ions, we have used the Rice-Ramsperger-Kassel-Marcus theory with the potential surfaces obtained from the ab initio quantum chemical calculations.
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