High harmonic generation and molecular orbital tomography in multielectron systems: beyond the single active electron approximation

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DOIResolve DOI: http://doi.org/10.1103/PhysRevLett.97.123003
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TypeArticle
Journal titlePhysical Review Letters
Volume97
Issue12
Pages1230034; # of pages: 123000
AbstractIt was recently shown that the highest molecular orbital of N2 could be reconstructed from a series of high harmonic measurements. Existing theories of high harmonic generation and orbital tomographic imaging are based on the single active electron approximation that ignores essential quantum mechanical properties such as the indistinguishability of identical particles and the Pauli exclusion principle. We show that, when fully antisymmetrized multielectron wave functions and electronic relaxation in the cation are considered, molecular orbital tomography records the image of the Dyson orbital plus exchange contributions from inner shells. The mixing of contributions from more than one molecular orbital gives access to additional wave function information. By utilizing the exchange term, harmonic emission from a closed-shell 4-electron system can be interpreted as a complete Hartree-Fock wave function.
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AffiliationNational Research Council Canada
Peer reviewedYes
NPARC number12328441
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Record identifier9b8cee8a-7945-4be7-b847-90191dff7f7e
Record created2009-09-10
Record modified2016-05-09
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