Imaging the electronic structure of valence orbitals in the XUV ionization of aligned molecules

We present measurements of photoelectron angular distributions (PADs) for the ionization of aligned CO2 molecules by an extreme ultraviolet laser pulse (17-45 eV) that is produced via high-harmonic generation, and that is polarized perpendicularly to the alignment laser axis. Differential PADs are r...

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Bibliographic Details
Published in:Journal of physics. B, Atomic, molecular, and optical physics Atomic, molecular, and optical physics, 2014-06, Vol.47 (12), p.1-9
Main Authors: Rouzée, Arnaud, Harvey, Alex G, Kelkensberg, Freek, Brambila, Danilo, Siu, Wing Kiu, Gademann, Georg, Smirnova, Olga, Vrakking, Marc J J
Format: Article
Language:English
Subjects:
Ab initio calculations
aligned molecules
Alignment
Angular distribution
Atomic and molecular physics
Autoionization, photoionization, and photodetachment
Calculations and mathematical techniques in atomic and molecular physics (excluding electron correlation calculations)
Carbon dioxide
Electronic structure
Electronic structure of atoms, molecules and their ions: theory
Exact sciences and technology
extreme ultraviolet
Frequency conversion
harmonic generation, including high-order harmonic generation
Fundamental areas of phenomenology (including applications)
Ionization
Lasers
Mathematical analysis
Molecular properties and interactions with photons
Molecular structure
Nonlinear optics
Optics
photoionization
Photon interactions with molecules
Physics
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Summary:We present measurements of photoelectron angular distributions (PADs) for the ionization of aligned CO2 molecules by an extreme ultraviolet laser pulse (17-45 eV) that is produced via high-harmonic generation, and that is polarized perpendicularly to the alignment laser axis. Differential PADs are recorded by taking the difference between two measurements for aligned and anti-aligned molecules. The results are compared with ab initio multi-channel R-matrix calculations, which are extended to include the computation of PADs. The calculations agree very well with the experiment, and are resolved with respect to the internal state of the ion and the polarization of the ionizing laser field relative to the molecular frame. For a sufficiently high, but experimentally achievable degree of alignment, the nodal structure of the molecular orbital becomes visible in the PAD.
ISSN:0953-4075
1361-6455
DOI:10.1088/0953-4075/47/12/124017