Imaging orbitals with attosecond and Ångström resolutions: toward attochemistry? Imaging orbitals with attosecond and Ångström resolutions: toward attochemistry?

Pascal Salières 1 A Maquet 2 Stefan Haessler 3 J Caillat 2 R Taïeb 2
1 SPAM - Service des Photons, Atomes et Molécules
2 LCPMR - Laboratoire de Chimie Physique - Matière et Rayonnement
3 Photonics Institute
Abstract : The recently developed attosecond light sources make the investigation of ultrafast processes in matter possible with unprecedented time resolution. It has been proposed that the very mechanism underlying the attosecond emission allows the imaging of valence orbitals with Ångström space resolution. This controversial idea together with the possibility of combining attosecond and Ångström resolutions in the same measurements has become a hot topic in strong-field science. Indeed , this could provide a new way to image the evolution of the molecular electron cloud during , e. g. a chemical reaction in ' real time '. Here we review both experimental and theoretical challenges raised by the implementation of these prospects. In particular , we show how the valence orbital structure is encoded in the spectral phase of the recombination dipole moment calculated for Coulomb scattering states , which allows a tomographic reconstruction of the orbital using first-order corrections to the plane-wave approach. The possibility of disentangling multi-channel contributions to the attosecond emission is discussed as well as the necessary compromise between the temporal and spatial resolutions. (Some figures may appear in colour only in the online journal)
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Pascal Salières, A Maquet, Stefan Haessler, J Caillat, R Taïeb. Imaging orbitals with attosecond and Ångström resolutions: toward attochemistry? Imaging orbitals with attosecond and Ångström resolutions: toward attochemistry?. Reports on Progress in Physics, IOP Publishing, 2012, 75, pp.062401. ⟨10.1088/0034-4885/75/6/062401⟩. ⟨hal-01164756⟩

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