Self-imaging of molecules from diffraction spectra by laser-induced rescattering electrons

Xu, Junliang; Chen, Zhangjin; Le, Anh-Thu; Lin, C. D.

doi:10.1103/physreva.82.033403

Cited by 73 publications

(96 citation statements)

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“…This result can be used to extend the range of applicability of ultrafast imaging techniques such as laser-induced electron diffraction and for the accurate characterization of laser pulses. DOI: 10.1103/PhysRevA.95.031402 With the advent of few-cycle intense laser technology, ultrafast imaging techniques such as laser-induced electron diffraction (LIED) [1][2][3][4][5][6][7][8][9][10][11][12] and high-order harmonic spectroscopy (HHS) [13][14][15][16][17][18][19] have recently been proposed. These techniques have been demonstrated to be capable of imaging molecular structural changes with unprecedented subangstrom spatial and few-femtosecond temporal resolutions [10,11,14,19].…”

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Retrieval of target structure information from laser-induced photoelectrons by few-cycle bicircular laser fields

Hoang

Lin

et al. 2017

Phys. Rev. A

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By analyzing theoretical results from a numerical solution of the time-dependent Schrödinger equation for atoms in few-cycle bicircular laser pulses, we show that high-energy photoelectron momentum spectra can be used to extract accurate elastic scattering differential cross sections of the target ion with free electrons. We find that the retrieval range for a scattering angle with bicircular pulses is wider than with linearly polarized pulses, although the retrieval method has to be modified to account for different returning directions of the electron in the continuum. This result can be used to extend the range of applicability of ultrafast imaging techniques such as laser-induced electron diffraction and for the accurate characterization of laser pulses. DOI: 10.1103/PhysRevA.95.031402 With the advent of few-cycle intense laser technology, ultrafast imaging techniques such as laser-induced electron diffraction (LIED) [1][2][3][4][5][6][7][8][9][10][11][12] and high-order harmonic spectroscopy (HHS) [13][14][15][16][17][18][19] have recently been proposed. These techniques have been demonstrated to be capable of imaging molecular structural changes with unprecedented subangstrom spatial and few-femtosecond temporal resolutions [10,11,14,19]. Both these techniques are based on the rescattering physics [20,21] with linearly polarized laser pulses.Quite recently, efficient high-order harmonic generation with bicircular pulses has been achieved [22,23], which provides a new tabletop circularly polarized coherent extreme ultraviolet to soft x-ray source with photon energies up to 160 eV [24]. Subsequently, these harmonics have been demonstrated to be very sensitive to electronic structure [25][26][27][28][29][30][31]. Clearly, in a bicircular pulse, after tunneling ionization from the target, the electron in the continuum is driven in a two-dimensional (2D) plane of the laser polarizations, instead of being confined to the laser polarization direction, as in the linearly polarized case. This fact has been utilized by Mancuso et al. [32] as a way to decouple the electron tunneling angle from the rescattering angle. Mancuso et al. found that this decoupling in turn leads to the separation of rescattered electrons in the low-energy region, in contrast to the linearly polarized case, where they are normally contaminated by the direct electrons.Previous experimental studies of electron spectra in bicircular laser fields have been mostly limited to the low-energy region so far [32,33]. On the theory side, both low-and high-energy regions have been studied by the strong-field approximation (SFA) [34,35] as well as the classical trajectory Monte Carlo method [33]. However, these works mainly focused on a comparison with experiments at low energies [33] or analyzing the SFA results in terms of the quantum orbit theory [34,35].In this Rapid Communication, based on the numerical solution of the time-dependent Schrödinger equation (TDSE) for different atoms in few-cycle bicircular laser pulses, we show that high-energy ph...

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Retrieval of target structure information from laser-induced photoelectrons by few-cycle bicircular laser fields

Hoang

Lin

et al. 2017

Phys. Rev. A

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“…However the recollision energies are around a few tens of eV, too small to resolve the atomic core positions necessary for molecular imaging (see Refs. [11,17]). In this Letter, we report high-resolution photoelectron momentum distributions of rare-gas atoms recorded at midinfrared (MIR) wavelengths (>1 m) which generate recollision energies approaching 300 eV.…”

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Laser-Induced Electron Diffraction for Probing Rare Gas Atoms

Blaga

DiChiara

et al. 2012

Phys. Rev. Lett.

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Recently, using midinfrared laser-induced electron diffraction (LIED), snapshots of a vibrating diatomic molecule on a femtosecond time scale have been captured [C. I. Blaga et al., Nature (London) 483, 194 (2012)]. In this Letter, a comprehensive treatment for the atomic LIED response is reported, a critical step in generalizing this imaging method. Electron-ion differential cross sections (DCSs) of rare gas atoms are extracted from measured angular-resolved, high-energy electron momentum distributions generated by intense midinfrared lasers. Following strong-field ionization, the high-energy electrons result from elastic rescattering of a field-driven wave packet with the parent ion. For recollision energies !100 eV, the measured DCSs are indistinguishable for the neutral atoms and ions, illustrating the close collision nature of this interaction. The extracted DCSs are found to be independent of laser parameters, in agreement with theory. This study establishes the key ingredients for applying LIED to femtosecond molecular imaging. DOI: 10.1103/PhysRevLett.109.233002 PACS numbers: 33.20.Xx, 33.60.+q, 34.80.Bm, 34.80.Qb An atom exposed to an intense low-frequency laser pulse can tunnel ionize, releasing an electron. Born in the laser's oscillating field, the electron may be accelerated back to recollide with the parent ion [1,2], incurring various electron-ion collision processes, such as elastic and inelastic scattering, and photorecombination. The recollision event is the basis of the strong-field rescattering model, which describes phenomena such as high-energy above-threshold ionization (HATI), nonsequential ionization, and high-harmonic generation. The combined elements of elastic scattering occurring on an optical-cycle time scale, e.g., femtoseconds, inherent in this model has generated interest in exploiting this as an ultrafast structural probe [3], analogous to diffraction using electron beams [4,5]. The viability of this self-imaging technique, dubbed laser-induced electron diffraction (LIED), has been addressed by several theoretical [6][7][8][9] and experimental [10,11] studies. A key principle was established by the quantitative rescattering (QRS) theory [7]: the field-free large-angle electron-ion (e-ion) elastic differential cross section (DCS) can be retrieved from a measured HATI electron momentum distribution. However in order for LIED to become an effective ultrafast imaging method, it is necessary that the valence (outer-shell) electrons of the target, e.g., molecules, play no significant role in the elastic process since their rearrangement which induces structural dynamics, i.e., motion of nuclei, is de facto unknown, and thus their interaction with the recolliding electron cannot be characterized.Underpinning the concept of imaging via LIED is the ability to produce high-energy core-penetrating e-ion recollisions. Previous studies [12][13][14][15][16] using 0:8 m laser pulses have demonstrated the capability of extracting DCSs from atoms and molecules. However the recollision energ...

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“…LIED features can be interpreted with the semianalytical models provided by the quantitative rescattering theory. According to the quantitative rescattering theory [71,72,74], photoelectrons are released by tunnel ionization with an initial velocity of near zero. They then quiver in the laser field before returning back towards the target ion with incident momentum k 0 where they scatter elastically in all directions with scattered momentum k r (|k r | = |k 0 |).…”

Section: Fullerenementioning

confidence: 99%

Efficient and accurate modeling of electron photoemission in nanostructures with TDDFT

2017

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Abstract. We review different computational methods for the calculation of photoelectron spectra and angular distributions of atoms and molecules when excited by laser pulses using time-dependent density-functional theory (TDDFT) that are suitable for the description of electron emission in compact spatial regions. We derive and extend the time-dependent surface-flux method introduced in Reference [1] within a TDDFT formalism and compare its performance to other existing methods. We illustrate the performance of the new method by simulating strong-field ionization of C 60 fullerene and discuss final state effects in the orbital reconstruction of planar organic molecules.

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Self-imaging of molecules from diffraction spectra by laser-induced rescattering electrons

Cited by 73 publications

References 60 publications

Retrieval of target structure information from laser-induced photoelectrons by few-cycle bicircular laser fields

Retrieval of target structure information from laser-induced photoelectrons by few-cycle bicircular laser fields

Laser-Induced Electron Diffraction for Probing Rare Gas Atoms

Efficient and accurate modeling of electron photoemission in nanostructures with TDDFT

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