Laser-Induced Electron Tunneling and Diffraction

Meckel, M.; Comtois, D.; Zeidler, D.; Staudte, A.; Pavičić, Domagoj; Bandulet, H.; Pépin, H.; Kieffer, Jean‐Claude; Dørner, R.; Villeneuve, D. M.; Corkum, P. B.

doi:10.1126/science.1157980

Cited by 742 publications

(533 citation statements)

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“…This phenomenon, 'laser-induced recollision', enables new measurement techniques: photorecombination leads to attosecond pulse production [9] whereas elastic and inelastic electron rescattering offer new approaches to diffraction imaging. [2,10,11] In typical experiments, the electron has acquired up to 100 eV of kinetic energy during its transit in the continuum and can release it in the form of an attosecond pulse. Since the emission takes place around each zero-crossing of the field, the described mechanism generates a train of attosecond pulses separated by half the period of the generating laser field.…”

Section: Introductionmentioning

confidence: 99%

High-Harmonic Spectroscopy: From Femtosecond to Attosecond Molecular Dynamics

Wörner

2011

Chimia

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The principles of high-harmonic spectroscopy (HHS) are illustrated using two recent examples from the literature. The method can be applied as a probe to measure the evolution of the electronic structure of a molecule during a chemical reaction on the femtosecond time scale. Alternatively, it can be used as a comprehensive method unifying pump and probe steps into a single laser cycle to measure electronic dynamics on the at to second time scale.

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Section: Introductionmentioning

confidence: 99%

High-Harmonic Spectroscopy: From Femtosecond to Attosecond Molecular Dynamics

Wörner

2011

Chimia

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“…This would also allow us to compare the alignment dependence of single-photon PI by soft X-ray with multiphoton ionization by IR lasers [194,195]. In Sec.…”

Section: Introductionmentioning

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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“…Combining conventional electron or X-ray beam methods with femtosecond laser pulses provides improved temporal resolutions for molecular dynamics investigation approaching atomic time scales [23][24][25][26] . However, recent experiments [27][28][29][30][31] demonstrated that intense, isolated femtosecond pulses alone are sufficient for imaging simple molecules via a strong-field three-step process 32,33 (see Supplementary Discussion). First, the intense, low-frequency laser ionizes the molecule.…”

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confidence: 99%

“…Conceptually this is analogous to the external electron beam used in conventional electron diffraction (CED) studies. Dubbed laser-induced electron diffraction (LIED) 34,35 , the method relies on extracting elastic differential cross-sections (DCS) from the two-dimensional (2D) photoelectron angular distributions [27][28][29][30][31] . Recently, picometre and femtosecond resolutions were demonstrated for N 2 and O 2 bond distance determination by fitting the extracted angledependent elastic DCS 36 .…”

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confidence: 99%

Diffraction using laser-driven broadband electron wave packets

Blaga

Zhang

et al. 2014

Nat Commun

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Directly monitoring atomic motion during a molecular transformation with atomic-scale spatio-temporal resolution is a frontier of ultrafast optical science and physical chemistry. Here we provide the foundation for a new imaging method, fixed-angle broadband laser-induced electron scattering, based on structural retrieval by direct one-dimensional Fourier transform of a photoelectron energy distribution observed along the polarization direction of an intense ultrafast light pulse. The approach exploits the scattering of a broadband wave packet created by strong-field tunnel ionization to self-interrogate the molecular structure with picometre spatial resolution and bond specificity. With its inherent femtosecond resolution, combining our technique with molecular alignment can, in principle, provide the basis for time-resolved tomography for multi-dimensional transient structural determination.

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Laser-Induced Electron Tunneling and Diffraction

Cited by 742 publications

References 34 publications

High-Harmonic Spectroscopy: From Femtosecond to Attosecond Molecular Dynamics

High-Harmonic Spectroscopy: From Femtosecond to Attosecond Molecular Dynamics

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

Diffraction using laser-driven broadband electron wave packets

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