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We present the application of ultrafast time- and mass-resolved ion yield laser spectroscopy in conjunction with ab initio electronic structure calculations to track molecular excited-state dynamics. We discuss how molecular fragment ions can be associated with conformations the molecule assumes during its relaxation, and how various features of the pump-probe signal for those fragments can be used...
We use an acousto-optic modulator at the input to a two-dimensional, Fourier-domain pulse shaper to achieve built-in characterization of the output pulses with spectral interferometry. The device is capable of rapid switching between pulse shapes.
We demonstrate an improved acousto-optic modulator for ultrafast optical pulse shaping making use of a diamond shaped transducer. Measurements of the spatial profile of the diffracted light beam agree well with Fresnel diffraction calculations.
We investigate dissociative ionization of aligned N2 molecules using intense ultrafast laser pulses. We find surprising differences in the yields of N2++, N+(1, 0) and N+(1, 1) as a function of molecular axis-laser polarization angle.
We measure the dependence of molecular fragmentation on a simple pulse shape parameterization at different intensities. The results indicate that dynamic Stark shifts of intermediate resonances play an important role in closed loop learning control.
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