2009
DOI: 10.1103/physrevlett.102.073902
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Elliptically Polarized High-Order Harmonic Emission from Molecules in Linearly Polarized Laser Fields

Abstract: We perform an accurate polarimetry measurement of high-order harmonic emission from aligned molecules. We find that harmonic emission from N2 can be strongly elliptically polarized even when driven by linearly polarized laser fields. These data have broad implications for understanding molecules in strong fields because they cannot be explained by simple theories based on the strong field approximation and single active electron models. Finally, this work also shows that it is possible to engineer the polariza… Show more

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Cited by 217 publications
(152 citation statements)
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References 23 publications
(23 reference statements)
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“…It has also been observed in N 2 that orbitals lying energetically below the HOMO, in particular the HOMO-1, also contribute to HHG in molecules [20]. Recent theoretical and experimental studies of the HHG polarization provide additional support for multiorbital effects [52][53][54]. The experimental phase determined for N 2 may have both HOMO and HOMO-1 contributions.…”
mentioning
confidence: 91%
“…It has also been observed in N 2 that orbitals lying energetically below the HOMO, in particular the HOMO-1, also contribute to HHG in molecules [20]. Recent theoretical and experimental studies of the HHG polarization provide additional support for multiorbital effects [52][53][54]. The experimental phase determined for N 2 may have both HOMO and HOMO-1 contributions.…”
mentioning
confidence: 91%
“…Figure 2 presents then the evolution of the normalized intensity The ellipticity of each harmonic in the two-colour configuration is evaluated from equation (1), which will be derived below. First, the ellipticity can be expressed as follows 17 assuming that e is small, which is naturally correct at Brewster's angle:…”
Section: Methodsmentioning
confidence: 99%
“…Several methods were proposed to overcome this restriction [8][9][10][11][12][13][14][15][16] , but only three of them really show the production of high harmonics with elliptical polarization and non-negligible efficiency. The first possibility consists in generating harmonics in pre-aligned molecules [17][18][19] . In this approach, however, the measured ellipticity can hardly exceed 35% and only for harmonics corresponding to the low efficiency part of the generated spectrum.…”
mentioning
confidence: 99%
“…High-order harmonic radiation is coherent with welldefined polarization [14]. We can write the emitted radiation field E em (t) as…”
Section: Harmonic Polarizationmentioning
confidence: 99%
“…The direction of greatest emission corresponds to the main polarization direction, and the emission in the orthogonal direction is a measure for the ellipticity of the emitted radiation [14]. Only under considerable effort for the experimentalist, the harmonic phase can be measured interferometrically as a function of alignment angle [10,23] or as a function of harmonic order [24].…”
Section: Harmonic Polarizationmentioning
confidence: 99%