Attosecond Time-Resolved Imaging of Molecular Structure by Photoelectron Holography

Bian, Xue-Bin; Bandrauk, André D.

doi:10.1103/physrevlett.108.263003

Cited by 134 publications

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“…its frequency. Because of their high energy, in contrast with that of direct electrons which is 2U p , RE can be used as signal and DE as reference to image atomic and molecular structure by photoelectron holography [20,25].Compared to atoms, the study of strong-field electron dynamics in molecules, in particular ionization, offers a richer perspective due to the additional degrees of freedom associated with the nuclei. Indeed, several phenomena due to the multicenter character of the molecular potential have already been discovered, such as charge-resonanceenhanced ionization [26] and light-induced-electron diffraction [27][28][29].…”

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confidence: 99%

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Correlated Electron and Nuclear Dynamics in Strong Field Photoionization ofH2+

et al. 2013

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We present a theoretical study of H þ 2 ionization under strong IR femtosecond pulses by using a method designed to extract correlated (2D) photoelectron and proton kinetic energy spectra. The results show two distinct ionization mechanisms-tunnel and multiphoton ionization-in which electrons and nuclei do not share the energy from the field in the same way. Electrons produced in multiphoton ionization share part of their energy with the nuclei, an effect that shows up in the 2D spectra in the form of energy-conservation fringes similar to those observed in weak-field ionization of diatomic molecules. In contrast, tunneling electrons lead to fringes whose position does not depend on the proton kinetic energy. At high intensity, the two processes coexist and the 2D plots show a very rich behavior, suggesting that the correlation between electron and nuclear dynamics in strong field ionization is more complex than one would have anticipated. DOI: 10.1103/PhysRevLett.110.113001 PACS numbers: 33.20.Xx, 33.60.+q, 33.80.Rv The interaction of atoms and molecules with intense infrared laser pulses has been the object of continuous research for more than two decades [1][2][3][4][5][6][7][8][9]. Since the potential induced by such lasers on the electrons is comparable to or even stronger than that generated by the nuclei, the resulting electron dynamics is significantly different from that of the isolated system, which makes these lasers ideal tools to achieve electronic control [10][11][12][13]. Strong fields can efficiently excite and ionize atoms and molecules. The electrons, which can be ejected following either multiphoton absorption or tunneling, can either directly reach the detector after having been repeatedly accelerated and decelerated by the field [direct electrons (DE)] or recollide with the ionic core within an optical cycle [rescattered electrons (RE)] [14,15]. Only a small fraction of the ejected electrons rescatter, but this fraction is responsible for important nonlinear phenomena such as high-harmonic generation (HHG). In this process, high-energy photons are emitted as a result of electron recombination with the ionic core. HHG is currently used to produce ultrashort extreme ultraviolet laser pulses and trains of these pulses [16][17][18][19], and also to uncover multielectron dynamics in atoms and molecules [13,20] or the structure of atomic and molecular orbitals in the so-called orbital tomography [10,21,22].Rescattered electrons that do not recombine with the ion also leave their signature in the photoelectron spectra at relatively high energies, typically between 2U p and 10U p [23,24], where U p ¼ I=4! 2 is the electron ponderomotive energy (in a.u.), I is the laser intensity, and ! its frequency. Because of their high energy, in contrast with that of direct electrons which is 2U p , RE can be used as signal and DE as reference to image atomic and molecular structure by photoelectron holography [20,25].Compared to atoms, the study of strong-field electron dynamics in molecules, in particular ...

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Correlated Electron and Nuclear Dynamics in Strong Field Photoionization ofH2+

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“…Eq. (10) shows that in general these two processes interfere for a given asymptotic electron momentum (k x , k y ). It has been shown that large electron energies (and thus small de Broglie wavelengths able to resolve sub-Å spatial scales) are reached by electrons ionized around a maximum of the field [26].…”

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confidence: 99%

“…Since then, several theoretical and experimental LIED related studies were performed in order to image time-resolved dynamics of molecular systems [5][6][7][8][9]. Closely related to LIED is the attosecond photoelectron holography imaging idea, again pioneered by A. D. Bandrauk and coworkers [10,11].…”

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Laser-induced electron diffraction: inversion of photo-electron spectra for molecular orbital imaging

et al. 2017

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In this paper, we discuss the possibility of imaging molecular orbitals from photoelectron spectra obtained via Laser Induced Electron Diffraction (LIED) in linear molecules. This is an extension of our work published recently in Physical Review A 94, 023421 (2016) to the case of the HOMO-1 orbital of the carbon dioxide molecule. We show that such an imaging technique has the potential to image molecular orbitals at different internuclear distances in a sub-femtosecond time scale and with a resolution of a fraction of an Angström.

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“…With the development of the laser technology, the interaction between the intense laser pulses and the atoms [1,2] or the molecules [3,4] becomes an issue of wide interest and has received a lot of attention. High-order harmonic generation (HHG) as one of the most important nonlinear phenomena has been investigated for many years due to its potential applications in the generation of coherent UV attosecond pulses [5,6] and in the time-resolved dynamics measurement of the atomic/molecular structure [7].…”

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Role of Excited States in Asymmetric Harmonic Emission

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2013

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Abstract:Role of excited states is theoretically studied in the asymmetric harmonic generation from quasi-asymmetric molecule LiH 3+ . The calculated energies and time-dependent populations on the relevant electron states demonstrate that there is the laser-induced electron transfer between the ground state and the first few excited states, which is responsible for the observed multiple frequencies enhancements on the harmonic emission process. In addition, such electron transfer process is very likely to be general for the quasi-asymmetric molecules, as suggested by calculations for LiH 3+ at different internuclear distances and with different central frequencies, pulse intensities, carrier-envelope phases, pulse durations as well as for the other quasi-asymmetric molecule BeH 4+ .

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Attosecond Time-Resolved Imaging of Molecular Structure by Photoelectron Holography

Cited by 134 publications

References 17 publications

Correlated Electron and Nuclear Dynamics in Strong Field Photoionization ofH2+

Correlated Electron and Nuclear Dynamics in Strong Field Photoionization ofH2+

Laser-induced electron diffraction: inversion of photo-electron spectra for molecular orbital imaging

Role of Excited States in Asymmetric Harmonic Emission

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