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Investigation of changing molecular orbitals using high-harmonic radiation tomography with resolving the full two dimensonal phase map


In this work pictures of the highest occupied orbital of changing molecular states will be taken using the molecular orbital tomography technique. This technique is based on the harmonic radiation emitted by the aligned sample molecules interacting with a strong IR-laser field. From amplitude, polarization and relative phases of the harmonic radiation the molecular orbital involved in the process can be reconstructed. The molecular orbital tomography has an intrinsic time resolution of below one femtosecond, which allows resolving very fast nuclear and electronic dynamics. For the first time, two detection schemes, one by two color photoionization and one by high harmonic interferometry will be combined to measure the complete phase map without using any assumptions for the phase relations between different molecular alignments or different harmonics. With this optimized detection scheme, the changes of a molecular orbital during a chemical reaction will be investigated. Two different reactions will be investigated during this work: the photodissociation of N2O and the photoisomerization of vinylidene (H2CC) to acetylene (HCCH). In this processes the initial molecular state is not inversion symmetric, therefore the typical used molecular alignment technique is not sufficient, it can not select between the two possible molecular orientations N2O or ON2, a much more complicated molecular orientation schemes will be used instead.

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Rue Leblanc 25
75015 Paris 15
Activity type
Research Organisations
EU contribution
€ 194 064
Administrative Contact
Jean-Christophe Coste (Mr.)