Multiorbital Tunneling Ionization of the CO Molecule

Wu, Jian; Schmidt, L. Ph. H.; Kunitski, Maksim; Meckel, M.; Voss, S.; Sann, H.; Kim, H.; Jahnke, T.; Czasch, A.; Dørner, R.

doi:10.1103/physrevlett.108.183001

Cited by 165 publications

(141 citation statements)

References 37 publications

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“…It is the convolution of the momentum distributions of two sequentially removed electrons. As first and second electron can both be emitted either in + y or − y direction, the combination yields four possible sum momenta 27,28,31 as indicated with the orange bars in Fig. 3a (see Methods).…”

Section: Resultsmentioning

confidence: 99%

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Probing the tunnelling site of electrons in strong field enhanced ionization of molecules

Meckel

Schmidt

et al. 2012

Nat Commun

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molecules show a much increased multiple ionization rate in a strong laser field as compared with atoms of similar ionization energy. A widely accepted model attributes this to the action of the joint fields of the adjacent ionic core and the laser on its neighbour inside the same molecule. The underlying physical picture for the enhanced ionization is that it is the up-field atom that gets ionized. However, this is still debated and remains unproven. Here we report an experimental verification of this long-standing prediction. This is accomplished by probing the two-site double ionization of ArXe, where the instantaneous field direction at the moment of electron release and the emission direction of the correlated ionizing centre are measured by detecting the recoil sum-and relative-momenta of the fragment ions. our results unambiguously prove the intuitive picture of the enhanced multielectron dissociative ionization of molecules and clarify a long-standing controversy.

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Section: Resultsmentioning

confidence: 99%

“…streaking' [24][25][26][27][28][29][30] . Hence, the field direction at the instant of ionization is mapped to the momentum direction of the released electron.…”

Section: Resultsmentioning

confidence: 99%

Probing the tunnelling site of electrons in strong field enhanced ionization of molecules

Meckel

Schmidt

et al. 2012

Nat Commun

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“…Recently, a few experiments have started addressing the role of a nonisotropic Coulomb potential and the electronic structure on molecular photoelectron distributions by studying strongfield ionization of molecules [24][25][26][27][28][29][30]. In these experiments, strong deviations of the measured radial and angular photoelectron spectra compared to the predictions from the strong-field approximation were found.…”

Section: Introductionmentioning

confidence: 97%

Classical analysis of Coulomb effects in strong-field ionization of H2+by intense circularly polarized laser fields

et al. 2013

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Vous avez des questions? Nous pouvons vous aider. Pour communiquer directement avec un auteur, consultez la première page de la revue dans laquelle son article a été publié afin de trouver ses coordonnées. Si vous n'arrivez pas à les repérer, communiquez avec nous à PublicationsArchive-ArchivesPublications@nrc-cnrc.gc.ca. Questions? Contact the NRC Publications Archive team atPublicationsArchive-ArchivesPublications@nrc-cnrc.gc.ca. If you wish to email the authors directly, please see the first page of the publication for their contact information. NRC Publications Archive Archives des publications du CNRCThis publication could be one of several versions: author's original, accepted manuscript or the publisher's version. / La version de cette publication peut être l'une des suivantes : la version prépublication de l'auteur, la version acceptée du manuscrit ou la version de l'éditeur. NRC Publications Record / Notice d'Archives des publications de CNRC:http://nparc.cisti-icist.nrc-cnrc.gc.ca/eng/view/object/?id=5bc1d097-91ab-4942-a161-98e52a911b43 http://nparc.cisti-icist.nrc-cnrc.gc.ca/fra/voir/objet/?id=5bc1d097-91ab-4942-a161-98e52a911b43 We analyze the distortion of the molecular frame photoelectron angular distributions of H 2 + ionized by a strong, circularly polarized infrared laser field using classical trajectory Monte Carlo simulations. We find that the nonisotropic field of the molecular ion rotates the final electron momenta. The degree of distortion from the strong-field approximation's predictions is thereby sensitive to the field strength and the internuclear distance but, counterintuitively, does not necessarily decrease for high field strengths. Furthermore, the distortion also depends crucially on the initial momentum of the classical electron after tunneling, while the exact shape of the ionization rate seems to be less important. A trajectory analysis within our simple model allows us to interpret recent experimental results.

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“…For linearly polarized light, on the other hand, one experiment reports most ionization from the Send [88], while another most perpendicular to the molecular axis [89]. For the CO molecule, as another example, strong-field ionization experiments performed in the tun- neling regime report that ionization occurs most readily when the external field has a component pointing from the C-to the O-end, and the electron leaves from the C-end [90][91][92]. This is in contrast with the results from application [87,93] of SAE approximation tunneling theory [84], which predicts that ionization is most likely when the field points from the O-to the C-end.…”

Section: Strong-field Ionizationmentioning

confidence: 99%

Time-dependent generalized-active-space configuration-interaction approach to photoionization dynamics of atoms and molecules

2014

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We present a wave-function based method to solve the time-dependent many-electron Schrödinger equation (TDSE) with special emphasis on strong-field ionization phenomena. The theory builds on the configuration-interaction (CI) approach supplemented by the generalized-active-space (GAS) concept from quantum chemistry. The latter allows for a controllable reduction in the number of configurations in the CI expansion by imposing restrictions on the active orbital space. The method is similar to the recently formulated time-dependent restricted-active-space (TD-RAS) CI method [D. Hochstuhl, and M. Bonitz, Phys. Rev. A 86, 053424 (2012)]. We present details of our implementation and address convergence properties with respect to the active spaces and the associated account of electron correlation in both ground state and excitation scenarios. We apply the TD-GASCI theory to strong-field ionization of polar diatomic molecules and illustrate how the method allows us to uncover a strong correlation-induced shift of the preferred direction of emission of photoelectrons.

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Multiorbital Tunneling Ionization of the CO Molecule

Cited by 165 publications

References 37 publications

Probing the tunnelling site of electrons in strong field enhanced ionization of molecules

Probing the tunnelling site of electrons in strong field enhanced ionization of molecules

Classical analysis of Coulomb effects in strong-field ionization of H2+by intense circularly polarized laser fields

Time-dependent generalized-active-space configuration-interaction approach to photoionization dynamics of atoms and molecules

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