Coherent control of attosecond emission from aligned molecules

Boutu, Willem; Haessler, Stefan; Merdji, H.; Breger, P.; Waters, G.; Stankiewicz, Marek; Frasinski, L. J.; Taïeb, Richard; Caillat, Jérémie; Maquet, Alfred; Monchicourt, P.; Carré, B.; Salieres, P.

doi:10.1038/nphys964

Cited by 221 publications

(221 citation statements)

References 30 publications

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“…An amplitude minimum in the vicinity of q=21 and θ = 0 • , accompanied by a rapid local phase variation with increasing q, is observed experimentally. The position of this minimum (q=21) is consistent with the two-center interference model [28]; a similar feature around q=23 was also observed in the recombination dipole of aligned CO 2 measured by the RABBIT technique [7], Br 2 and CO 2 having the same ordering of valence molecular orbitals.…”

supporting

confidence: 82%

Linked attosecond phase interferometry for molecular frame measurements

et al. 2013

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supporting

confidence: 82%

Linked attosecond phase interferometry for molecular frame measurements

et al. 2013

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“…Using the plane-wave approximation, this should be a sharp π -phase jump [6]. However, in experiments a smaller and smoother phase jump is observed [20]. Such deviations can be attributed to nonclassical momenta [21] and to effects of the Coulombic potential [22].…”

Section: Harmonic Phasementioning

confidence: 95%

“…The phase jump in the x direction at the two-center interference minimum becomes smoother for low harmonics [20][21][22]. In the following we investigate how the jump in the polarization direction depends on harmonic order.…”

Section: A Polarization Directionmentioning

confidence: 99%

Two-center interference and ellipticity in high-order harmonic generation fromH2+

Zwan

Lein

2010

Phys. Rev. A

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We present a theoretical investigation into the two-center interference in aligned H + 2 . The influence of the laser field on the recombination step is investigated by comparing laser-induced harmonic generation with harmonic generation from field-free collisions of Gaussian wave packets with the core. We find that for different Gaussian wave packets colliding with the molecule, the interference minimum occurs at the same alignment angle. The same result is obtained for the laser-induced spectrum when only a single electronic trajectory per harmonic contributes. When multiple electronic trajectories contribute, we find an effect on the minimum position because the interference between short and long trajectories is alignment dependent. The two-center interference and the influence of the Coulombic potential are clearly seen not only in the harmonic intensity and phase but also in the polarization direction and ellipticity. We observe significant ellipticity of the emitted radiation around the two-center interference minimum.

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“…One advantage of studying HHG is that the phase of the dipole transition matrix element can be retrieved from the phase of the harmonics, see Refs. [95,102,165,168]. On the other hand, unlike photoionization, experimental HHG spectra suffer from macroscopic propagation effect as discussed in Chapter 6 and thus care must be taken when drawing conclusions on single molecule HHG spectra from experimental HHG spectra.…”

Section: Connection Between Photoionization and Harmonic Generationmentioning

confidence: 99%

Theory of Nonlinear Propagation of High Harmonics Generated in a Gaseous Medium

Jin

2013

Springer Theses

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In this thesis, we establish the theoretical tools to investigate high-order harmonic generation (HHG) by intense infrared lasers in a gaseous medium. The macroscopic propagation of both the fundamental and the harmonic fields is taken into account by solving Maxwell's wave equations, while the single-atom (or single-molecule) response is obtained by quantitative rescattering theory. The initial spatial mode of the fundamental laser is assumed either a Gaussian or a truncated Bessel beam. On the examples of Ar, N 2 and CO 2 , we demonstrate that the available experimental HHG spectra with isotropic and aligned target media can be accurately reproduced theoretically even though the HHG spectra are sensitive to the experimental conditions. We show that the macroscopic HHG can be expressed as a product of a macroscopic wave packet and a photorecombination cross section, where the former depends on laser and experimental conditions while the latter is the property of the target only. The factorization makes it possible to retrieve the single-atom or single-molecule structure information from experimental HHG spectra. As for the multiple molecular orbital contribution in HHG, it causes the disappearance of the minimum in the HHG spectrum of aligned N 2 with the increase of laser intensity, and the position of minimum in HHG spectrum of aligned CO 2 depending on many factors is also attributed to it, which could explain why the minima observed in different laboratories may differ. For an important application of HHG as ultrashort light source, we show that measured continuous harmonic spectrum of Xe due to the reshaping of the fundamental laser field can be used to produce an isolated attosecond pulse by spectral and spatial filtering in the far field. For on-going application of using HHG to ionize aligned molecules, we present the photoelectron angular distribution from aligned N 2 and CO 2 in the laboratory frame, which can be compared directly with future experiments. demonstrate that the available experimental HHG spectra with isotropic and aligned target media can be accurately reproduced theoretically even though the HHG spectra are sensitive to the experimental conditions. We show that the macroscopic HHG can be expressed as a product of a macroscopic wave packet and a photorecombination cross section, where the former depends on laser and experimental conditions while the latter is the property of the target only. The factorization makes it possible to retrieve the single-atom or single-molecule structure information from experimental HHG spectra. As for the multiple molecular orbital contribution in HHG, it causes the disappearance of the minimum in the HHG spectrum of aligned N 2 with the increase of laser intensity, and the position of minimum in HHG spectrum of aligned CO 2 depending on many factors is also attributed to it, which could explain why the minima observed in different laboratories may differ. For an important application of HHG as ultrashort light source, we show that measured continu...

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Coherent control of attosecond emission from aligned molecules

Cited by 221 publications

References 30 publications

Linked attosecond phase interferometry for molecular frame measurements

Linked attosecond phase interferometry for molecular frame measurements

Two-center interference and ellipticity in high-order harmonic generation fromH2+

Theory of Nonlinear Propagation of High Harmonics Generated in a Gaseous Medium

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