4.8 Article

Influence of orbital symmetry on diffraction imaging with rescattering electron wave packets

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NATURE COMMUNICATIONS
卷 7, 期 -, 页码 -

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NATURE PUBLISHING GROUP
DOI: 10.1038/ncomms11922

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资金

  1. Spanish Ministry of Economy and Competitiveness [FIS2014-56774-R, FIS2014-51478-ERC]
  2. 'Severo Ochoa' Programme for Centres of Excellence in RD [SEV-2015-0522]
  3. Catalan Agencia de Gestio d'Ajuts Universitaris i de Recerca (AGAUR) with SGR
  4. Fundacio Cellex Barcelona
  5. European Union's Horizon research and innovation programme [654148 Laserlab-Europe]
  6. Marie Sklodowska-Curie Grant [641272, 264666]
  7. COST Action [MP1203]
  8. COST Action XLIC
  9. ICFONEST programme - COFUND (FP7-PEOPLE- COFUND)
  10. AGAUR with a PhD fellowship (FI-DGR)
  11. Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy (DOE) [DE-FG02-86ER13491]
  12. ICREA Funding Source: Custom

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The ability to directly follow and time-resolve the rearrangement of the nuclei within molecules is a frontier of science that requires atomic spatial and few-femtosecond temporal resolutions. While laser-induced electron diffraction can meet these requirements, it was recently concluded that molecules with particular orbital symmetries (such as pi(g)) cannot be imaged using purely backscattering electron wave packets without molecular alignment. Here, we demonstrate, in direct contradiction to these findings, that the orientation and shape of molecular orbitals presents no impediment for retrieving molecular structure with adequate sampling of the momentum transfer space. We overcome previous issues by showcasing retrieval of the structure of randomly oriented O-2 and C2H2 molecules, with pi(g) and pi(u) symmetries, respectively, and where their ionization probabilities do not maximize along their molecular axes. While this removes a serious bottleneck for laser-induced diffraction imaging, we find unexpectedly strong backscattering contributions from low-Z atoms.

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