Laser-driven electron recollision is at the heart of the rapidly growing field of attosecond science. The recollision wavepacket is qualitatively described within the strong-field approximation, ...which commonly assumes tunnelling ionization and plane-wave propagation of the liberated electron in the continuum. However, with increasing experimental sophistication, refinements to this simple model have become necessary. Through careful modelling and measurements of laser-induced recollision holography using aligned N2 molecules, we demonstrate that the continuum electron wavepacket already carries a non-trivial spatial phase structure immediately following ionization. This effect is of rather general character: any molecule and any non-isotropic system that is ionized by a strong laser field will exhibit an offset in the phase of the continuum electron wavepacket. Specifically, this has important implications for any coherent scattering process in molecules, such as high-harmonic generation or laser-induced electron holography.
It is well established that electrons can escape from atoms through tunneling under the influence of strong laser fields, but the timing of the process has been controversial and far too rapid to ...probe in detail. We used attosecond angular streaking to place an upper limit of 34 attoseconds and an intensity-averaged upper limit of 12 attoseconds on the tunneling delay time in strong field ionization of a helium atom. The ionization field derives from 5.5-femtosecond-long near-infrared laser pulses with peak intensities ranging from 2.3 x 10¹⁴ to 3.5 x 10¹⁴ watts per square centimeter (corresponding to a Keldysh parameter variation from 1.45 to 1.17, associated with the onset of efficient tunneling). The technique relies on establishing an absolute reference point in the laboratory frame by elliptical polarization of the laser pulse, from which field-induced momentum shifts of the emergent electron can be assigned to a temporal delay on the basis of the known oscillation of the field vector.
Electron motion on the (sub-)femtosecond time scale constitutes the fastest response in many natural phenomena such as light-induced phase transitions and chemical reactions. Whereas static electron ...densities in single molecules can be imaged in real space using scanning tunnelling and atomic force microscopy, probing real-time electron motion inside molecules requires ultrafast laser pulses. Here, we demonstrate an all-optical approach to imaging an ultrafast valence electron wave packet in real time with a time-resolution of a few femtoseconds. We employ a pump-probe-deflect scheme that allows us to prepare an ultrafast wave packet via strong-field ionization and directly image the resulting charge oscillations in the residual ion. This approach extends and overcomes limitations in laser-induced orbital imaging and may enable the real-time imaging of electron dynamics following photoionization such as charge migration and charge transfer processes.
Laser-Induced Electron Tunneling and Diffraction Meckel, M; Comtois, D; Zeidler, D ...
Science (American Association for the Advancement of Science),
06/2008, Letnik:
320, Številka:
5882
Journal Article
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Molecular structure is usually determined by measuring the diffraction pattern the molecule impresses on x-rays or electrons. We used a laser field to extract electrons from the molecule itself, ...accelerate them, and in some cases force them to recollide with and diffract from the parent ion, all within a fraction of a laser period. Here, we show that the momentum distribution of the extracted electron carries the fingerprint of the highest occupied molecular orbital, whereas the elastically scattered electrons reveal the position of the nuclear components of the molecule. Thus, in one comprehensive technology, the photoelectrons give detailed information about the electronic orbital and the position of the nuclei.
Tunneling, one of the most striking manifestations of quantum mechanics, influences the electronic structure of many molecules and solids and is responsible for radioactive decay. Much of the ...interaction of intense light pulses with matter commences with electrons tunneling from atoms or molecules to the continuum. Until recently, this starting point was assumed to be the highest occupied orbital of a given system. We have now observed tunneling from a lower-lying state in hydrogen chloride (HCl). Analyzing two independent experimental observables allowed us to isolate (via fragment ions), identify (via molecular frame photoelectron angular distributions), and, with the help of ab initio simulations, quantify the contribution of lower-lying orbitals to the total and angle-dependent tunneling current of the molecule. Our results bolster the emerging tenet that the coherent interaction between different orbitals--which can amplify the impact of lower orbitals--must be considered in tunneling processes.
The strong coupling between intense laser fields and valence electrons in molecules causes distortions of the potential energy hypersurfaces which determine the motion of the nuclei and influence ...possible reaction pathways. The coupling strength varies with the angle between the light electric field and valence orbital, and thereby adds another dimension to the effective molecular potential energy surface, leading to the emergence of light-induced conical intersections. Here, we demonstrate that multiphoton couplings can give rise to complex light-induced potential energy surfaces that govern molecular behavior. In the laser-induced dissociation of H
, the simplest of molecules, we measure a strongly modulated angular distribution of protons which has escaped prior observation. Using two-color Floquet theory, we show that the modulations result from ultrafast dynamics on light-induced molecular potentials. These potentials are shaped by the amplitude, duration and phase of the dressing fields, allowing for manipulating the dissociation dynamics of small molecules.
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