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M Wollenhaupt

Publications and source records attributed to M Wollenhaupt.

4 recordsLinked to original sources

Femtosecond laser photoelectron spectroscopy on atoms and small molecules: prototype studies in quantum control.

We review prototype studies in the area of quantum control with femtosecond lasers. We restrict this discussion to atoms and diatomics under gas-phase collision-free conditions to allow for a comparison between theory and experiment. Both the perturbative regime and the nonperturbative regime of the light-matter interaction are addressed. To that end, atomic/molecular beam techniques are combined together with femtosecond laser techniques and energy-resolved photoelectron spectroscopy and ion detection. Highly detailed information on the laser-induced quantum dynamics is extracted with the help of kinetic energy-resolved photoelectron spectroscopy.

Ions↗

Quantum control by ultrafast polarization shaping.

We demonstrate that the use of time-dependent light polarization opens a new level of control over quantum systems. With potassium dimer molecules from a supersonic molecular beam, we show that a polarization-shaped laser pulse increases the ionization yield beyond that obtained with an optimally shaped linearly polarized laser pulse. This is due to the different multiphoton ionization pathways in K2 involving dipole transitions which favor different polarization directions of the exciting laser field. This experiment is a qualitative extension of quantum control mechanisms which opens up new directions giving access to the three-dimensional temporal response of molecular systems.

Journal Article↗

Interferences of ultrashort free electron wave packets.

Interferences of free electron wave packets generated by a pair of identical, time-delayed, femtosecond laser pulses which ionize excited atomic potassium have been observed. Two different schemes are investigated: threshold electrons produced by one-photon ionization with parallel laser polarization and above threshold ionization electrons produced by a two-photon transition with crossed laser polarization. Our results show that the temporal coherence of light pulses is transferred to free electron wave packets, thus opening the door to a whole variety of exciting experiments.

Journal Article↗

The position dependent 15N enrichment of nitrous oxide in the stratosphere.

The position dependent 15N fractionation of nitrous oxide (N2O), which cannot be obtained from mass spectrometric analysis on molecular N2O itself, can be determined with high precision using isotope ratio mass spectrometry on the NO+ fragment that is formed on electron impact in the source of an isotope ratio mass spectrometer. Laboratory UV photolysis experiments show that strong position dependent 15N fractionations occur in the photolysis of N2O in the stratosphere, its major atmospheric sink. Measurements on the isotopic composition of stratospheric N2O indeed confirm the presence of strong isotope enrichments, in particular the difference in the fractionation constants for 15N14NO and 14N15NO. The absolute magnitudes of the fractionation constants found in the stratosphere are much smaller, however, than those found in the lab experiments, demonstrating the importance of dynamical and also additional chemical processes like the reaction of N2O with O(1D).

Air Pollutants↗