Twin Markovian field correlation on four-level attosecond polarization beats

Based on the phase-conjugate polarization interference between two two-photon processes, we obtained an analytic closed form for the second-order or fourth-order Markovian stochastic correlation of the four-level attosecond sum-frequency polarization beat (FASPB) in the extremely Doppler-broadened limit. The homodyne-detected FASPB signal is shown to be particularly sensitive to the statistical properties of the Markovian stochastic light fields with arbitrary bandwidth. The different roles of the amplitude fluctuations and the phase fluctuations can be understood physically in the time-domain picture. The field correlation has a weak influence on the FASPB signal when the laser has narrow bandwidth. In contrast, when the laser has broadband linewidth, the FASPB signal shows resonant-nonresonant cross-correlation, and drastic difference for three Markovian stochastic fields. The maxima of the two two-photon signals are shifted from zero time delay to the opposite direction, and the signal exhibits damping oscillation when the laser frequency is off-resonant from the two-photon transition. A Doppler-free precision in the measurement of the energy-level sum can be achieved with an arbitrary bandwidth. As an attosecond ultrafast modulation process, it can be extended intrinsically to any sum frequency of energy levels.

A velocity map ion-imaging study on C2H5SH and C3H7SH photodissociation at 243 nm

Photodissociation dynamics Of C2H5SH, i-C-3-H7SH and n-C3H7SH at 243.1 nm were investigated using velocity map ion-imaging method. H-atom photolysis products were detected by a (2 + 1) resonance enhanced ionization scheme. Both the angular distribution and translational energy distribution of the H-atom elimination processes were determined from the ion images of the H-atom products. The experimental results indicate that the H-atom eliminations from these molecules are mainly direct and fast dissociation processes from a repulsive potential energy state. And a more statistical dissociation process that likely occurs oil the ground state via internal conversion has also been observed. Dissociation energies of the S-H bonds are also derived from the H-atom product translational energy distributions. (C) 2002 Elsevier Science B.V. All rights reserved.