High Harmonic Generation and Molecular Orbital Tomography in Multielectron Systems: Beyond the Single Active Electron Approximation

Patchkovskii, Serguei; Zhao, Zengxiu; Brabec, Thomas; Villeneuve, D. M.

doi:10.1103/physrevlett.97.123003

Cited by 174 publications

(63 citation statements)

References 18 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…This error is also observed in the previous works especially for the σ orbital. Besides the limited spectrum range, the imaging errors may also result from several other reasons, such as the discrete sampling in the frequency domain with the interval of 2ω L , and the SFA and singleactive-electron approximation used in the theoretical model [7][8][9][10]12]. In the MOT process, when the Stark phase is approximately subtracted by using the analytical expression derived in [18], the main structure of the target orbital is also successfully reproduced in both the length and velocity forms.…”

Section: Tomographic Reconstructionmentioning

confidence: 95%

“…By applying this method to a series of aligned molecules, they accomplished a tomographic reconstruction of the highest occupied molecular orbital (HOMO) of N 2 . Since then, the MOT has attracted a great deal of attention for its great significance in uncovering the basic properties of molecules and chemical reactions [7][8][9][10][11][12][13]. In most of the works, the target molecular orbitals are symmetric with either gerade or ungerade symmetry, while the MOT of nonsymmetric orbitals is more difficult.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Influence of large permanent dipoles on molecular orbital tomography

Zhu¹,

Qin²,

Zhang³

et al. 2013

Opt. Express

View full text Add to dashboard Cite

The influence of large permanent dipoles on molecular orbital tomography via high-order harmonic generation (HHG) is investigated in this work. It is found that, owing to the modification of the angle-dependent ionization rate resulting from the Stark shift, the one-side-recollision condition for the tomographic imaging can not be satisfied even with the few-cycle driving pulses. To overcome this problem, we employ a tailored driving pulse by adding a weak low-frequency pulse to the few-cycle laser pulse to control the HHG process and the recollision of the continuum electrons are effectively restricted to only one side of the core. Then we carried out the orbital reconstruction in both the length and velocity forms. The results show that, the orbital structure can only be successfully reproduced by using the dipole matrix elements projected perpendicular to the permanent dipole in both forms.

show abstract

Section: Tomographic Reconstructionmentioning

confidence: 95%

Section: Introductionmentioning

confidence: 99%

Influence of large permanent dipoles on molecular orbital tomography

Zhu¹,

Qin²,

Zhang³

et al. 2013

Opt. Express

View full text Add to dashboard Cite

show abstract

“…Different channels of ionization can thus be expected to play role, as well as the electron-electron correlations [147,148].…”

Section: High Harmonic Generation: Multielectron Effectsmentioning

confidence: 99%

“…Works on the role of electron exchange and spin statistics of electrons in the molecule [147,148] showed that molecular orbital tomography, first described in [92], reconstructs the Dyson orbital of the molecule together with the effects of the electron correlations, imaging signatures of lower orbital as well as HOMO. Dyson orbital is an overlap between the wave function of the ground…”

Section: High Harmonic Generation: Multielectron Effectsmentioning

confidence: 99%

Multidimensional high harmonic spectroscopy

Serbinenko

Smirnova

2013

2013 Conference on Lasers &Amp; Electro-Optics Europe &Amp; International Quantum Electronics Conference CLEO EUROPE/IQEC

View full text Add to dashboard Cite

Multidimensional high harmonic spectroscopy is a cutting-edge technique for studying the effect of the intense low-frequency laser fields on atoms and molecules. The high energy photons, emitted by a particle as a result of the interaction with the strong laser field, carry the information about the processes in atoms and molecules, which lead to the emission. Multidimensional character of the technique allows to extract parameters of the molecular and atomic ionization dynamics, that were inaccessible before in the same experiment, such as sub-cycle ionization rates, ionization and recombination times.The Thesis presents in detail theoretical analysis of the multidimensional high harmonic generation process within semi-classical approach. Several generating field configurations are considered. The developed theoretical apparatus is then applied to describe multidimensional high harmonic spectroscopy experiments in helium. Initial analysis of the applicability of the technique for the study of multielectron dynamics in carbon dioxide is also performed.The problems, solutions to which are presented in the Thesis, are:• theoretical description of high harmonic generation in multicolor fields• analysis of the gating techniques for the extraction of the parameters of electron trajectories in high harmonic generation in He• proposition of an alternative reconstruction procedure of electron trajectory parameters, that allows one to access to all of them simultaneouslyThe main results of our work are:• Based on theoretical analysis of multidimensional high harmonic generation, we showed, that optimization of the two-dimensional harmonic 3 signal is achieved at each step of the process: ionization, propagation, dynamics in the ion and recombination• We demonstrated, that multidimensional high harmonic spectroscopy is a very sensitive tool allowing one to extract parameters of electron trajectories, such as complex ionization time and complex electron momentum, from the observed harmonic signal• We developed and applied theory to the analysis of two-color high harmonic generation experiments of He atom• We performed initial analysis of two-color HHG experiments in carbon dioxide, which was necessary for further investigation and reconstruction I thank Bettina Becker, the most helpful person in the institute or in the whole world, who made the bureaucratic problems very easy. There was no question she didn't answer and no problem she didn't solve quickly and efficiently.

show abstract

“…There has been a focus on diatomic molecules because of their relative simplicity and the ability to align them relative to the laser polarization [7]. For the case of single-photon ionization, or recombination leading to harmonic emission, it was shown that the measurements reflect the Dyson orbital associated with the ionization [8]. In the case of tunnel ionization of groundstate diatomic molecules, while there is no direct formalism that relates the angle-resolved ionization yields to the molecular orbital structure, the ionization yield as a function of the angle between the laser polarization vector and the molecular axis has been shown to reflect the shape of the orbital from which an electron was removed, i.e., the hole left following ionization [9][10][11][12].…”

Section: Introductionmentioning

confidence: 99%

Strong-Field Molecular Ionization from Multiple Orbitals

et al. 2011

View full text Add to dashboard Cite

We demonstrate strong-field ionization from multiple orbitals of excited-state uracil molecules. The molecules are excited to the first bright state by an ultrafast laser pulse in the deep ultraviolet and then ionized with a strong-field laser pulse in the near infrared during ultrafast relaxation back down to the ground state. We measure time-and angle-dependent ion yields for multiple fragments created by strongfield ionization, and interpret the temporally and angularly resolved yields via ab initio electronic structure calculations. We find that the angular distribution for the electron removed from the lowest unoccupied molecular orbital follows the symmetry of the molecular orbital, whereas ionization of the molecule by removing electrons from deeper bound orbitals is more complicated.

show abstract

High Harmonic Generation and Molecular Orbital Tomography in Multielectron Systems: Beyond the Single Active Electron Approximation

Cited by 174 publications

References 18 publications

Influence of large permanent dipoles on molecular orbital tomography

Influence of large permanent dipoles on molecular orbital tomography

Multidimensional high harmonic spectroscopy

Strong-Field Molecular Ionization from Multiple Orbitals

Contact Info

Product

Resources

About