Transient enhancement of high-order harmonic generation in expanding molecules

Pfeifer, Thomas; Walter, Dominik; Gerber, G.; Emelin, M. Yu.; Ryabikin, M. Yu.; Chernobrovtseva, M. D.; Sergeev, A.

doi:10.1103/physreva.70.013805

Cited by 28 publications

(26 citation statements)

References 23 publications

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“…The time-dependent Schrödinger equation was solved using a split-step operator approach [18][19][20]. The internuclear wave-packet evolution |Ψ(R, t c )| 2 is shown in The pump-probe KER spectra N (E KER , τ ) can now be calculated by using Eq.…”

Section: (A)mentioning

confidence: 99%

Noisy Optical Pulses Enhance the Temporal Resolution of Pump-Probe Spectroscopy

et al. 2012

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Time-resolved measurements of quantum dynamics are based on the availability of controlled events (e.g. pump and probe pulses) that are shorter in duration than the typical evolution time scale of the dynamical processes to be observed. Here we introduce the concept of noise-enhanced pump-probe spectroscopy, allowing the measurement of dynamics significantly shorter than the average pulse duration by exploiting randomly varying, partially coherent light fields consisting of bunched colored noise. It is shown that statistically fluctuating fields can be superior by more than a factor of 10 to frequency-stabilized fields, with important implications for time-resolved pump-probe experiments at x-ray free-electron lasers (FELs) and, in general, for measurements at the frontiers of temporal resolution (e.g. attosecond spectroscopy). As an example application, the concept is used to explain the recent experimental observation of vibrational wave-packet motion in a deuterium molecular ion on time scales shorter than the average pulse duration.

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Section: (A)mentioning

confidence: 99%

Noisy Optical Pulses Enhance the Temporal Resolution of Pump-Probe Spectroscopy

et al. 2012

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“…It consists in preliminary excitation and ionization of molecules by an ultrashort optical pulse of small intensity followed by the action on the gas by a high-power radiation pulse whose time delay corresponds to optimal "swelling" of the molecule in the course of its oscillations or started dissociation. The sequential action on the molecule by two pulses, the pump pulse (the electronic-vibrational excitation of the molecule) and the probing pulse with a varied time delay (harmonic generation), can be used as a diagnostic tool for observing the nonlinear-response dynamics related to intramolecular structural changes [31].…”

Section: Molecular Sizes and Configurationmentioning

confidence: 99%

Possibilities for controlling attosecond x-ray pulse generation during molecular ionization by femtosecond laser radiation

Emelin

Ryabikin

Sergeev

2004

Radiophys Quantum Electron

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UDC 539.19We discuss the role of different factors (molecular sizes and configuration, orientation of the molecular axis with respect to the electric field of a laser pulse, the type of the molecular orbital, etc.), which characterize molecules and their state, in the formation of the nonlinear response of a molecule ionized by a high-power femtosecond laser pulse. In numerical experiments within the framework of a two-dimensional model for the H + 2 molecular ion, we study possibilities for controlling the process of nonlinear frequency conversion of femtosecond optical radiation into Xray radiation of attosecond duration by means of preliminary vibrational or electronic excitation of molecules. We demonstrate the possibilities of using the attosecond pulse generation as a diagnostic tool for probing vibration-rotational dynamics of molecules.

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“…In part, this is motivated by the potential for HHG from 1 molecules to be a new avenue for attosecond pulse production with additional control knobs compared with atoms. For instance it has been shown that molecular alignment can modulate HHG yield [1,2] and that the internuclear separation and electronic state character can significantly alter the wave-packet dynamics, which lead to the formation of even shorter attosecond radiation bursts from the HHG process from the molecules than found in atoms [3]. It was also recently shown that the alignment dependence of the harmonic spectra can be used to reconstruct the molecular orbital [2].…”

Section: Introductionmentioning

confidence: 98%

Molecular orbital dependence of high-order harmonic generation

Marangos

Altucci

Velotta

et al. 2006

Journal of Modern Optics

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We examine the role of the electronic orbital of a molecule in the process of high-order harmonic generation. To do this, measurements of high-order harmonic generation in molecules (O 2 , N 2 , H 2 , CO 2 and small alkanes) and atoms (Xe, Ar and Kr) have been carried out with intense fewoptical-cycle pulses. Comparison between molecules and their 'companion' atoms (i.e. those with nearly equal ionization potential) was made. The molecule response in the high-field regime is treated by adopting an 'atom-like' model for the forms of the molecular orbitals employing the Lewenstein et al. model, properly modified in order to account for the nonlinear dipole moment of a randomly oriented molecule ensemble. The calculation procedure is described here in detail. There is good agreement between the spectra calculated using this model and the harmonic cut-off position and the shape of the measured spectra. The cut-offs of O 2 and CO 2 extend far beyond the cut-offs of Xe and Kr respectively, in contrast with N 2 and H 2 which exhibit cutoffs very close to that of Ar. This behaviour is well explained by adopting the atom-like approximation. A series of alkanes has also been investigated and again the spectra are well matched by this simple model.

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Transient enhancement of high-order harmonic generation in expanding molecules

Cited by 28 publications

References 23 publications

Noisy Optical Pulses Enhance the Temporal Resolution of Pump-Probe Spectroscopy

Noisy Optical Pulses Enhance the Temporal Resolution of Pump-Probe Spectroscopy

Possibilities for controlling attosecond x-ray pulse generation during molecular ionization by femtosecond laser radiation

Molecular orbital dependence of high-order harmonic generation

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