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- Klünder, Kathrin, et al.
(author)
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Reconstruction of attosecond electron wave packets using quantum state holography
- 2013
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In: Physical Review A (Atomic, Molecular and Optical Physics). - 1050-2947. ; 88:3
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Journal article (peer-reviewed)abstract
- We present a method for performing quantum state holography, with which we completely characterize the amplitude and phase of an attosecond electron wave packet. Our approach is an extension of a recent publication [J. Mauritsson et al., Phys. Rev. Lett. 105, 053001 (2010)] in which we demonstrated experimentally that the energies and amplitudes of an attosecond electron wave packet can be characterized using attosecond electron interferometry. Here we show theoretically that attosecond electron interferometry can be extended to retrieve the phases of all the states that make up the wave packet. We demonstrate the feasibility of our method by analyzing a wave packet created by a shake-up process. We show that our method can successfully retrieve arbitrary phases and/or lifetimes added to the component eigenstates.
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- Mauritsson, Johan, et al.
(author)
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Attosecond Electron Spectroscopy Using a Novel Interferometric Pump-Probe Technique
- 2010
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In: Physical Review Letters. - 1079-7114. ; 105:5
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Journal article (peer-reviewed)abstract
- We present an interferometric pump-probe technique for the characterization of attosecond electron wave packets (WPs) that uses a free WP as a reference to measure a bound WP. We demonstrate our method by exciting helium atoms using an attosecond pulse (AP) with a bandwidth centered near the ionization threshold, thus creating both a bound and a free WP simultaneously. After a variable delay, the bound WP is ionized by a few-cycle infrared laser precisely synchronized to the original AP. By measuring the delay-dependent photoelectron spectrum we obtain an interferogram that contains both quantum beats as well as multipath interference. Analysis of the interferogram allows us to determine the bound WP components with a spectral resolution much better than the inverse of the AP duration.
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- Sansone, G., et al.
(author)
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Electron localization following attosecond molecular photoionization
- 2010
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In: Nature. - : Springer Science and Business Media LLC. - 0028-0836 .- 1476-4687. ; 465:7299, s. 3-763
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Journal article (peer-reviewed)abstract
- For the past several decades, we have been able to directly probe the motion of atoms that is associated with chemical transformations and which occurs on the femtosecond (10(-15)-s) timescale. However, studying the inner workings of atoms and molecules on the electronic timescale(1-4) has become possible only with the recent development of isolated attosecond (10(-18)-s) laser pulses(5). Such pulses have been used to investigate atomic photoexcitation and photoionization(6,7) and electron dynamics in solids(8), and in molecules could help explore the prompt charge redistribution and localization that accompany photoexcitation processes. In recent work, the dissociative ionization of H-2 and D-2 was monitored on femtosecond timescales(9) and controlled using few-cycle near-infrared laser pulses(10). Here we report a molecular attosecond pump-probe experiment based on that work: H-2 and D-2 are dissociatively ionized by a sequence comprising an isolated attosecond ultraviolet pulse and an intense few-cycle infrared pulse, and a localization of the electronic charge distribution within the molecule is measured that depends-with attosecond time resolution-on the delay between the pump and probe pulses. The localization occurs by means of two mechanisms, where the infrared laser influences the photoionization or the dissociation of the molecular ion. In the first case, charge localization arises from quantum mechanical interference involving autoionizing states and the laser-altered wavefunction of the departing electron. In the second case, charge localization arises owing to laser-driven population transfer between different electronic states of the molecular ion. These results establish attosecond pump-probe strategies as a powerful tool for investigating the complex molecular dynamics that result from the coupling between electronic and nuclear motions beyond the usual Born-Oppenheimer approximation.
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