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Ning, Qi-Cheng; Peng, Liang-You; Song, Shu-Na; Jiang, Wei-Chao; Nagele, Stefan; Pazourek, Renate; Burgdörfer, Joachim; Gong, Qihuang

doi:10.1103/physreva.90.013423

Cited by 38 publications

(34 citation statements)

References 62 publications

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“…18) as signatures of the destructive interference. The EWS time shift near Cohen-Fano interference minima is found not only sensitively dependent on the internuclear distance but also on the alignment angle of the molecular axis relative to the ionizing XUV pulse and the IR streaking field (Ning et al, 2014). For its observation, control over the molecular alignment is important.…”

Section: Time-resolved Photoionization Of Moleculesmentioning

confidence: 96%

“…The time encoded in the wavepacket of the receding electron carries information on the initial localization within the molecule as well on the near-field of neighboring atomic constituents. The simplest prototypical case is the photoionization of a diatomic molecule (Fernández et al, 2007;Hu et al, 2009;Guan et al, 2011;Ivanov et al, 2012;Bian and Bandrauk, 2012;Serov et al, 2013;Carpeggiani et al, 2014;Ning et al, 2014;Chacon et al, 2014). Among the fundamental questions to be addressed are: Does it take a longer time for the electron to escape from the multicenter molecular core than from the one-center atomic core?…”

Section: Time-resolved Photoionization Of Moleculesmentioning

confidence: 99%

“…This structural similarity implies, however, that the experimental observation may face a similar challenge as peaks in the EWS time shift are associated with (near) zero emission probability. First realistic simulations of an attosecond streaking setting (Ning et al, 2014) indicate that averaging over the radial distribution, ( ), of the molecule to be photoionized,…”

Section: Time-resolved Photoionization Of Moleculesmentioning

confidence: 99%

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Attosecond chronoscopy of photoemission

2015

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Recent advances in the generation of well characterized sub-femtosecond laser pulses have opened up unpredicted opportunities for the real-time observation of ultrafast electronic dynamics in matter. Such attosecond chronoscopy allows a novel look at a wide range of fundamental photophysical and photochemical processes in the time domain, including Auger and autoionization processes, photoemission from atoms, molecules, and surfaces, complementing conventional energy-domain spectroscopy. Attosecond chronoscopy raises fundamental conceptual and theoretical questions as which novel information becomes accessible and which dynamical processes can be controlled and steered. These questions are currently a matter of lively debate which we address in this review. We will focus on one prototypical case, the chronoscopy of the photoelectric effect by attosecond streaking. Is photoionization instantaneous or is there a finite response time of the electronic wavefunction to the photoabsorption event? Answers to this question turn out to be far more complex and multi-faceted than initially thought. They touch upon fundamental issues of time and time delay as observables in quantum theory. We review recent progress of our understanding of time-resolved photoemission from atoms, molecules, and solids. We will highlight the unresolved and open questions and we point to future directions aiming at the observation and control of electronic motion in more complex nanoscale structures and in condensed matter.

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Section: Time-resolved Photoionization Of Moleculesmentioning

confidence: 96%

Section: Time-resolved Photoionization Of Moleculesmentioning

confidence: 99%

Section: Time-resolved Photoionization Of Moleculesmentioning

confidence: 99%

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Attosecond chronoscopy of photoemission

2015

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“…Ning et al have investigated the simplest, prototypical molecule, H + 2 , and found * These two authors contributed equally. † E-mail: Alexander.Schubert@uni-jena.de pronounced interference effects (Cohen-Fano interferences, [14]) caused by the two scattering centers [15]. However, this prototype case inherently does not involve any multi-electron effects.…”

Section: Introductionmentioning

confidence: 99%

The impact of electron–electron correlation in ultrafast attosecond single ionization dynamics

Fröbel

Ziems

Peschel

et al. 2020

J. Phys. B: At. Mol. Opt. Phys.

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The attosecond ultrafast ionization dynamics of correlated two-or many-electron systems have, so far, been mainly addressed investigating atomic systems. In the case of single ionization, it is well known that electronelectron correlation modifies the ionization dynamics and observables beyond the single active electron picture, resulting in effects such as the Auger effect or shake-up/down and knock-up/down processes. Here, we extend these works by investigating the attosecond ionization of a molecular system involving correlated two-electron dynamics, as well as non-adiabatic nuclear dynamics. Employing a charge-transfer molecular model system with two differently bound electrons, a strongly and a weakly bound electron, we distinguish different pathways leading to ionization, be it direct ionization or ionization involving elastic and inelastic electron scattering processes. We find that different pathways result in a difference in the electronic population of the parent molecular ion, which, in turn, involves different subsequent (non-adiabatic) postionization dynamics on different time scales.

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“…In contrast, a theory for molecular photoionization delays has not been developed so far, although calculations of such delays have been performed for H 2 and H + 2 , taking advantage of the analytical form of two-center Coulomb functions [25][26][27][28]. Very interesting insight has also been obtained from one-dimensional model systems [29,30].…”

mentioning

confidence: 99%

Attosecond delays in molecular photoionization

Hupperrt

Jordan

Baykusheva

et al. 2017

2017 Conference on Lasers and Electro-Optics Europe &Amp; European Quantum Electronics Conference (CLEO/Europe-EQEC)

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We report measurements of energy-dependent attosecond photoionization delays between the two outer-most valence shells of N2O and H2O. The combination of single-shot signal referencing with the use of different metal foils to filter the attosecond pulse train enables us to extract delays from congested spectra. Remarkably large delays up to 160 as are observed in N2O, whereas the delays in H2O are all smaller than 50 as in the photon-energy range of 20-40 eV. These results are interpreted by developing a theory of molecular photoionization delays. The long delays measured in N2O are shown to reflect the population of molecular shape resonances that trap the photoelectron for a duration of up to ∼110 as. The unstructured continua of H2O result in much smaller delays at the same photon energies. Our experimental and theoretical methods make the study of molecular attosecond photoionization dynamics accessible.Photoionization and photoelectron spectroscopies are powerful approaches to measuring the electronic structure of matter [1,2]. A complete quantum-mechanical description of photoionization, both in the time and frequency domains, requires the amplitude and phase of all dipole matrix elements, e.g. in a partial-wave expansion. Most experiments to date measure photoionization cross sections which are described by the sum of squared moduli of individual partial-wave dipole matrix elements. Cross sections thus contain no information about the partial-wave phase shifts. In contrast, photoelectron angular distributions are highly sensitive to partial-wave phase shifts [3,4] between continua associated with the same ionic state. Phase-shifts between continua associated with different ionization thresholds are not measurable in the frequency domain because the lack of spectral overlap between the corresponding photoelectrons erases the coherence required to measure such phase shifts.In this letter, we show that attosecond metrology can be employed to measure this information in molecular photoionization. Specifically, we study the effect of molecular shape resonances on the measured photoionization delays. When the combined molecular (or atomic) and centrifugal potential felt by the photoelectron displays a barrier, one or several quasi-bound states can emerge [5][6][7]. These resonances decay by tunneling through the potential barrier and often lead to a local enhancement of the photoionization cross section. Such shape resonances have so far only been measured by frequency-resolved measurements. Here, we show that attosecond metrology provides access to the time-domain manifestation of shape resonances. In the case of N 2 O, our measurements indeed reveal surprisingly large delays reaching up to 160 as in the range of 20 to 40 eV. In contrast, delays measured at the same photon energies in H 2 O all lie below 50 as in magnitude. These results are interpreted by developing a theory of molecular photoionization delays relying on accurate molecular scattering calculations. This analysis shows that the delays measured ...

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Attosecond streaking of Cohen-Fano interferences in the photoionization ofH2+

Cited by 38 publications

References 62 publications

Attosecond chronoscopy of photoemission

Attosecond chronoscopy of photoemission

The impact of electron–electron correlation in ultrafast attosecond single ionization dynamics

Attosecond delays in molecular photoionization

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