Quantitative rescattering theory of high-order harmonic generation for polyatomic molecules

Le, Anh-Thu; Lucchese, Robert R.; Lin, C. D.

doi:10.1103/physreva.87.063406

Cited by 37 publications

(49 citation statements)

References 43 publications

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“…For cis-DCE, the ionization yield is stronger when the field direction is closer to θ = 180 • , i.e., pointed away from the C-C center (or the electric force is closer to θ = 0 • , or pointed toward the C-C center). We comment that the angular dependence of the ionization rate looks very similar to that of the asymptotic wave function of the HOMO [21,28]. Overall, our angular dependence resembles the results of Spanner and Patchkovskii [29].…”

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confidence: 75%

“…(2) needs to be averaged over the isotropic molecular distribution [19,21]. A major advantage of this approach over the more standard approach of calculating the electron wave packet directly for the target using the strong-field approximation (SFA) is that it avoids possible spurious spikes, which occur quite frequently for polyatomic targets.…”

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confidence: 99%

“…In this Rapid Communication we employ the quantitative rescattering (QRS) theory [4,19,20] as extended to polyatomic targets [21] to calculate HHG spectra from cis and trans stereoisomers of 1,2-DCE and 2-butene under intense midinfrared laser pulses. Our calculation shows good agreements with experiment by Wong et al [16].…”

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confidence: 99%

“…1). Here, electron energy E is related to the emitted photon energy ω by E = ω − I p , with I p being the ionization potential of the target.We follow a version of the QRS in which a reference atom is used to calculate the energy-dependent returning electron wave packet, with the additional (alignment-dependent) phase η(θ,φ) approximated by the phase of the asymptotic initial wave function of the active electron [21],For the case of nonaligned molecules, Eq. (2) needs to be averaged over the isotropic molecular distribution [19,21].…”

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confidence: 99%

“…We follow a version of the QRS in which a reference atom is used to calculate the energy-dependent returning electron wave packet, with the additional (alignment-dependent) phase η(θ,φ) approximated by the phase of the asymptotic initial wave function of the active electron [21],…”

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High-order-harmonic generation from molecular isomers with midinfrared intense laser pulses

Lucchese

Lin

2013

Phys. Rev. A

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We present theoretical calculations of high-order-harmonic generation (HHG) from stereoisomers of 1,2-dichloroethylene (C 2 H 2 Cl 2 ) and 2-butene (C 4 H 8 ) based on the quantitative rescattering theory. Our results show that the HHG spectra from these cis and trans isomers with intense midinfrared laser pulses are clearly distinguishable, even when the molecules are randomly oriented, in good agreement with the recent experiments by Wong et al. [Phys. Rev. A 84, 051403(R) (2011)]. We found that the angle-averaged tunneling ionization yields and photoionization cross sections from the cis and trans isomers for both molecules are nearly identical. The origin of the differences in HHG spectra is traced as due to the interplay in the angular dependence of the photoionization (or photorecombination) cross section and ionization rate. High-order-harmonic generation (HHG) has been shown both experimentally and theoretically to contain information about the target molecular structure and dynamics, which are encoded in the amplitude and phase of the emitted high-order harmonics [1][2][3][4][5][6][7][8][9][10][11][12]. HHG spectroscopy for simple molecules has been greatly benefited from the ability to align molecules [13]. In fact, rich information contained in HHG spectra from aligned molecules is mostly washed out if the molecules are not well aligned. Whereas earlier studies have focused mostly on simple molecules with the use of infrared lasers, more recent studies in HHG spectroscopy have now expanded to more complex targets and by using midinfrared lasers [14][15][16][17].As the geometric arrangement of atoms in stereoisomers differs, they can serve as interesting tests for HHG spectroscopy. In a recent paper by Wong et al. [16], HHG spectra from stereoisomers of 1,2-dichloroethylene (1,2-DCE, C 2 H 2 Cl 2 ) and 2-butene (C 4 H 8 ) have been reported. It was found that the spectra from these cis and trans isomers are quite distinguishable in a broad range of energy, even when the molecules are not aligned. The mechanism behind this was attributed as due to the differences in the strong-field ionization. The ability to distinguish nonaligned isomers by HHG spectroscopy is of great interest. In particular, it opens up the possibility to study fast structural changes during the isomerization process using HHG [18] even without the need of molecular alignment.In this Rapid Communication we employ the quantitative rescattering (QRS) theory [4,19,20] as extended to polyatomic targets [21] to calculate HHG spectra from cis and trans stereoisomers of 1,2-DCE and 2-butene under intense midinfrared laser pulses. Our calculation shows good agreements with experiment by Wong et al. [16]. However, we found that the angle-averaged ionization yields from cis and trans isomers are nearly indistinguishable. Here we provide an analysis of the nature of the differences in HHG spectra from these isomers.Within the QRS, the laser-induced dipole D(ω,θ,φ) for a molecule in a linearly polarized intense laser pulse can be written as a p...

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confidence: 99%

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confidence: 99%

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confidence: 99%

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High-order-harmonic generation from molecular isomers with midinfrared intense laser pulses

Lucchese

Lin

2013

Phys. Rev. A

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Perspektiven für das Verständnis fundamentaler Elektronenkorrelationen durch Attosekundenspektroskopie

Kraus

Wörner

2018

Angewandte Chemie

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Zusammenfassung Molekülorbitale sind ein sehr erfolgreiches Konzept in der Chemie zur Beschreibung der elektronischen Struktur von Molekülen. Diese Beschreibung ist jedoch unzureichend, wenn die Elektronen in Molekülen stark korreliert sind und nicht als unabhängige Teilchen behandelt werden können. Die Auswirkungen solcher Elektronenkorrelationen sind allgegenwärtig in der Spektroskopie innerer Valenzelektronen durch Ultraviolet-und Röntgenstrahlen, ausserdem können Elektronenkorrelationen Ladungswanderungen in Molekülen vorantreiben und sind verantwortlich für viele exotische Eigenschaften stark korrelierter Materialien. Zeitaufgelöste Spektroskopie mit Attosekundenzeitauösung kann im Allgemeinen Elektronendynamik in Echtzeit verfolgen und kann dadurch einen experimentellen Zugang zu Phänomenen erönen, welche durch Elektronenkorrelation vorangetrieben werden. Die Spektroskopie hoher Harmonischer im Speziellen verwendet die präzise zeitabgestimmte Rekollision von laser-beschleunigten Elektronen, um die elektronische Struktur und Dynamik des untersuchten Systems auf einer sub-Femtosekunden Zeitskala zu messen. In diesem Übersichtsartikel diskutieren wir die Möglichkeiten der Spektroskopie hoher Harmonischer, um Elektronendynamik in Molekülen zu verfolgen. Wir besprechen, wie die Spektroskopie hoher Harmonischer auf qualitative und quantitative Weise analysiert werden kann, um die detaillierte Elektronendynamik in Molekülen nach Ionisierung zu verfolgen. Diese Fortschritte machen die Spektroskopie hoher Harmonischer zu einer vielversprechenden Methode, um fundamentale Elektronenkorrelationen aufzudecken und experimentelle Daten zu komplexen Elektronendynamiken bereitzustellen. * peter.kraus@berkeley.edu † hwoerner@ethz.ch; www.atto.ethz.ch 1

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Perspectives of Attosecond Spectroscopy for the Understanding of Fundamental Electron Correlations

Kraus

Wörner

2018

Angew Chem Int Ed

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The description of the electronic structure of molecules in terms of molecular orbitals is a highly successful concept in chemistry. However, it commonly fails if the electrons in a molecule are strongly correlated and cannot be treated as independent particles. Electron correlation is essential to understand inner-valence X-ray spectroscopies, it can drive ultrafast charge migration in molecules, and it is responsible for many exotic properties of strongly correlated materials. Time-resolved spectroscopy with attosecond resolution is generally capable of following electronic motion in real time and can thus provide experimental access to electron-correlation-driven phenomena. High-harmonic spectroscopy in particular uses the precisely timed laser-driven recollision of electrons to interrogate the electronic structure and dynamics of the investigated system on a sub-femtosecond timescale. In this Review, the capabilities of high-harmonic spectroscopy to follow electronic motion in molecules are discussed. Both qualitative and quantitative approaches to unraveling the detailed dynamical responses of molecular systems following ionization are presented. A new theoretical formalism for the reconstruction of correlation-driven charge migration is introduced. The importance of electron-ion entanglement and electronic coherence in the reconstruction of attosecond hole dynamics are discussed. These advances make high-harmonic spectroscopy a promising technique to decode fundamental electron correlations and to provide experimental data on the complex manifestations of multi-electron dynamics.

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Quantitative rescattering theory of high-order harmonic generation for polyatomic molecules

Cited by 37 publications

References 43 publications

High-order-harmonic generation from molecular isomers with midinfrared intense laser pulses

High-order-harmonic generation from molecular isomers with midinfrared intense laser pulses

Perspektiven für das Verständnis fundamentaler Elektronenkorrelationen durch Attosekundenspektroskopie

Perspectives of Attosecond Spectroscopy for the Understanding of Fundamental Electron Correlations

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