What is the effect of the Coulomb waves on the angular momentum?

For k<0.5 a.u., the fast oscillations in (c) are a direct imprint left by the Coulomb-waves, as can be seen from their partial wave-expansion37, where each angular momentum l contributes with a phase l(Z*,k) = arg[(l+1+iZ*/k)].

What is the velocity-form’ of the dipole?

Reconstructions in (b,d), are based on the `velocity-form’ of the dipole to avoid division by x/y in real space and thus numerical problems with the orbital nodes at y=0.

How was the relative timing calibration ensured?

2. Relative timing calibration was ensured by setting the group delay for the lowest harmonic (H17) to the same value for all angles (see Supplementary Information).

Why is the 150 as the overall time-shift between the measured and simulated pulse?

The ≈150 as overall time-shift between the measured (a) and simulated (b) pulse profiles is presumably due to macroscopic effects (dispersion during propagation), not accounted for in their simulations.

What is the setup for the RABITT?

Their setup is based on a Mach-Zehnder type interferometer for the `Reconstruction of AttosecondBeating by Interference of Two-photon Transitions’ (RABITT) measurement (see Supplementary Information).

What is the corresponding spectral intensity profile of an average pulse in the attosecond?

(a): Temporal intensity profile of an average pulse in the attosecond pulse train emitted by N2 molecules aligned at angles θ=0° to 90°, reconstructed from a series of RABITT measurements, taking into account harmonics 17 to 27.

Open AccessJournal Article10.1038/NPHYS1511

Attosecond imaging of molecular electronic wavepackets

Q: What have the authors contributed in "Attosecond imaging of molecular electronic wavepackets" ?

HAL this paper is a multi-disciplinary open access archive for the deposit and dissemination of scientific research documents, whether they are published or not.

Q: What is the effect of the laser pulse on the recombination of a gas?

HHG occurs when a strong laser pulse, of frequency L, tunnel-ionizes a gas target, creating an electron wave-packet (EWP) that is subsequently accelerated and driven back to the core where it recombines, emitting an attosecond burst of coherent soft X-rays18-20.

Q: What is the timescale of the attosecond electron-hole wave-packet?

The laser period being a few femtoseconds, the timescale of sub-cycle electron dynamics is attosecond, as in tunnelling ionization1,2 and continuum dynamics3-7.

Q: What is the polarization of the laser?

The generating laser is kept s-polarized while the molecular alignment axis is rotated in order to predominantly detect the HHG polarization component parallel to the driving laser.

Q: What is the effect of the Coulomb waves on the angular momentum?

For k<0.5 a.u., the fast oscillations in (c) are a direct imprint left by the Coulomb-waves, as can be seen from their partial wave-expansion37, where each angular momentum l contributes with a phase l(Z*,k) = arg[(l+1+iZ*/k)].

Q: What is the simplest way to obtain information on the attosecond wavepacket?

Both temporal and spatial information on this wavepacket can be obtained through the coherent soft X-ray emission resulting from the laserdriven recollision of the liberated electron with the core.

Q: What is the velocity-form’ of the dipole?

Reconstructions in (b,d), are based on the `velocity-form’ of the dipole to avoid division by x/y in real space and thus numerical problems with the orbital nodes at y=0.

Q: How was the relative timing calibration ensured?

2. Relative timing calibration was ensured by setting the group delay for the lowest harmonic (H17) to the same value for all angles (see Supplementary Information).

Q: Why is the 150 as the overall time-shift between the measured and simulated pulse?

The ≈150 as overall time-shift between the measured (a) and simulated (b) pulse profiles is presumably due to macroscopic effects (dispersion during propagation), not accounted for in their simulations.

Q: What is the setup for the RABITT?

Their setup is based on a Mach-Zehnder type interferometer for the `Reconstruction of AttosecondBeating by Interference of Two-photon Transitions’ (RABITT) measurement (see Supplementary Information).

Stefan Haessler, +11 more

- 01 Mar 2010

- Nature Physics

- Vol. 6, Iss: 3, pp 200-206

682

TL;DR: In this paper, the attosecond contributions of the two highest occupied molecular orbitals are analyzed and the conditions where they are disentangled in real and imaginary parts of the emission dipole moment are determined.

Abstract: A strong laser field may tunnel ionize a molecule from several orbitals simultaneously, forming an attosecond electron–hole wavepacket. Both temporal and spatial information on this wavepacket can be obtained through the coherent soft X-ray emission resulting from the laser-driven recollision of the liberated electron with the core. By characterizing the emission from aligned N 2 molecules, we demonstrate the attosecond contributions of the two highest occupied molecular orbitals. We determine conditions where they are disentangled in the real and imaginary parts of the emission dipole moment. This allows us to carry out a tomographic reconstruction of both orbitals with angstrom spatial resolution. Their coherent superposition provides experimental images of the attosecond wavepacket created in the ionization process. Our results open the prospect of imaging ultrafast intramolecular dynamics combining attosecond and angstrom resolutions.

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Most frequently asked questions

1. What have the authors contributed in "Attosecond imaging of molecular electronic wavepackets" ?

HAL this paper is a multi-disciplinary open access archive for the deposit and dissemination of scientific research documents, whether they are published or not.

2. What is the effect of the laser pulse on the recombination of a gas?

HHG occurs when a strong laser pulse, of frequency L, tunnel-ionizes a gas target, creating an electron wave-packet (EWP) that is subsequently accelerated and driven back to the core where it recombines, emitting an attosecond burst of coherent soft X-rays18-20.

3. What is the timescale of the attosecond electron-hole wave-packet?

The laser period being a few femtoseconds, the timescale of sub-cycle electron dynamics is attosecond, as in tunnelling ionization1,2 and continuum dynamics3-7.

4. What is the polarization of the laser?

The generating laser is kept s-polarized while the molecular alignment axis is rotated in order to predominantly detect the HHG polarization component parallel to the driving laser.

Citations

•Journal Article•10.1088/0953-4075/49/13/132001

Development of high harmonic generation spectroscopy of organic molecules and biomolecules

Jonathan P. Marangos

- 31 May 2016

- Journal of Physics B

TL;DR: In this article, the authors discuss the possibility to extract useful dynamical and structural information from the measurement of the HHG emission, a technique termed high harmonic generation spectroscopy (HHGS).

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Journal Article•10.1103/PHYSREVA.96.053406

Asymmetric molecular-orbital tomography by manipulating electron trajectories

Bincheng Wang, +6 more

- 09 Nov 2017

- Physical Review A

TL;DR: In this paper, a two-dimensional manipulation of the electron trajectories, the electrons can recollide with the target molecule from two noncollinear directions, and then the dipole moment generated from the single direction can be obtained to reconstructed the asymmetric molecular orbital.

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Journal Article•10.1063/1.5019356

Dissipation dynamics of field-free molecular alignment for symmetric-top molecules: Ethane (C2H6)

Haisu Zhang, +4 more

- 22 Mar 2018

- Journal of Chemical Physics

TL;DR: The field-free molecular alignment of symmetric-top molecules, ethane, induced by intense non-resonant linearly polarized femtosecond laser pulses is investigated experimentally and it is observed that the permanent alignment always decays slower compared to the transient alignment within the measured pressure range.

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Journal Article•10.1364/JOSAB.35.00A110

Ultrastable collinear delay control setup for attosecond IR-XUV pump–probe experiment

Amelle Zaïr, +3 more

- 01 May 2018

- Journal of The Optical Society of Americ...

TL;DR: In this article, a robust experimental design for performing time-resolved measurement with IR femtosecond laser pulses and attosecond extreme ultraviolet (XUV) pulses was presented.

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•Journal Article•10.1103/PHYSREVLETT.114.103004

Signatures of molecular orbital structure in lateral electron momentum distributions from strong-field ionization.

Ingo Petersen, +2 more

- 13 Mar 2015

- Physical Review Letters

TL;DR: It is demonstrated that orbital symmetries can be distinguished with the information obtained by observing the lateral width in addition to the angular distributions, by calculating the emission-angle-resolved lateral width of the momentum distribution perpendicular to the polarization plane.

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References

Journal Article•10.1002/JCC.540141112

General atomic and molecular electronic structure system

Michael W. Schmidt, +12 more

- 01 Nov 1993

- Journal of Computational Chemistry

TL;DR: A description of the ab initio quantum chemistry package GAMESS, which can be treated with wave functions ranging from the simplest closed‐shell case up to a general MCSCF case, permitting calculations at the necessary level of sophistication.

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•Journal Article•10.1103/PHYSREVLETT.71.1994

Plasma perspective on strong field multiphoton ionization.

Paul B. Corkum

- 27 Sep 1993

- Physical Review Letters

TL;DR: During strong-field multiphoton ionization, a wave packet is formed each time the laser field passes its maximum value, and one important parameter which determines the strength of these effects is the rate at which the wave packet spreads in the direction perpendicular to the laser electric field.

...read moreread less

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Journal Article•10.1103/revmodphys.81.163

Attosecond physics

Ferenc Krausz, +1 more

- 02 Feb 2009

- Reviews of Modern Physics

TL;DR: Attosecond physics explores the manipulation and tracking of atomic-scale electron motion using intense ultrashort light pulses.

...read moreread less

4.7K

Journal Article•10.1103/PHYSREVA.49.2117

Theory of high-harmonic generation by low-frequency laser fields.

Maciej Lewenstein, +4 more

- 01 Mar 1994

- Physical Review A

TL;DR: A simple, analytic, and fully quantum theory of high-harmonic generation by low-frequency laser fields is presented and the exact quantum-mechanical formula for the harmonic cutoff that differs from the phenomenological law Ip+3.17Up is presented.

...read moreread less

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Journal Article•10.1038/NATURE03183

Tomographic imaging of molecular orbitals

Jiro Itatani, +9 more

- 16 Dec 2004

- Nature

TL;DR: It is demonstrated that the full three-dimensional structure of a single orbital can be imaged by a seemingly unlikely technique, using high harmonics generated from intense femtosecond laser pulses focused on aligned molecules.

...read moreread less

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Attosecond imaging of molecular electronic wavepackets

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AI Agents for this Paper

Most frequently asked questions

1. What have the authors contributed in "Attosecond imaging of molecular electronic wavepackets" ?

2. What is the effect of the laser pulse on the recombination of a gas?

3. What is the timescale of the attosecond electron-hole wave-packet?

4. What is the polarization of the laser?

5. What is the effect of the Coulomb waves on the angular momentum?

6. What is the simplest way to obtain information on the attosecond wavepacket?

7. What is the velocity-form’ of the dipole?

8. How was the relative timing calibration ensured?

9. Why is the 150 as the overall time-shift between the measured and simulated pulse?

10. What is the setup for the RABITT?

11. What is the corresponding spectral intensity profile of an average pulse in the attosecond?

Citations

Development of high harmonic generation spectroscopy of organic molecules and biomolecules

Asymmetric molecular-orbital tomography by manipulating electron trajectories

Dissipation dynamics of field-free molecular alignment for symmetric-top molecules: Ethane (C2H6)

Ultrastable collinear delay control setup for attosecond IR-XUV pump–probe experiment

Signatures of molecular orbital structure in lateral electron momentum distributions from strong-field ionization.

References

General atomic and molecular electronic structure system

Plasma perspective on strong field multiphoton ionization.

Attosecond physics

Theory of high-harmonic generation by low-frequency laser fields.

Tomographic imaging of molecular orbitals

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