Orientation-dependent stereo Wigner time delay and electron localization in a small molecule

Vos, Jannie; Cattaneo, Laura; Patchkovskii, Serguei; Zimmermann, Tomáš; Cirelli, Claudio; Lucchini, Matteo; Kheifets, Anatoli; Landsman, Alexandra S.; Keller, U.

doi:10.1051/epjconf/201920506008

Cited by 30 publications

(39 citation statements)

References 12 publications

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“…The RABBIT technique has been widely used to determine accurate photoionization delays in atoms (20,21) and, following the pioneering work of Haessler et al (22), has started to be applied to molecular systems as well (23)(24)(25). Here, N 2 is ionized by a comb of odd high-order harmonics, covering the 3  g −1 shape resonance (see Fig.…”

Section: Resultsmentioning

confidence: 99%

Attosecond timing of electron emission from a molecular shape resonance

et al. 2020

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Shape resonances in physics and chemistry arise from the spatial confinement of a particle by a potential barrier. In molecular photoionization, these barriers prevent the electron from escaping instantaneously, so that nuclei may move and modify the potential, thereby affecting the ionization process. By using an attosecond two-color interferometric approach in combination with high spectral resolution, we have captured the changes induced by the nuclear motion on the centrifugal barrier that sustains the well-known shape resonance in valence-ionized N2. We show that despite the nuclear motion altering the bond length by only 2%, which leads to tiny changes in the potential barrier, the corresponding change in the ionization time can be as large as 200 attoseconds. This result poses limits to the concept of instantaneous electronic transitions in molecules, which is at the basis of the Franck-Condon principle of molecular spectroscopy.

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Section: Resultsmentioning

confidence: 99%

Attosecond timing of electron emission from a molecular shape resonance

et al. 2020

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“…Measurement techniques like reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) [6][7][8][9][10] and attosecond streaking [11,12] have made the relative Wigner time-delays τ W [13] between different orbitals of atoms and molecules accessible. Several pioneering experiments [6,11,12] have employed isolated attosecond pulses (IAP) and attosecond pulse trains (APTs) to resolve photoemission time-delays [13][14][15][16][17][18][19][20][21][22][23] in atoms, molecules and solids.…”

Section: Introductionmentioning

confidence: 99%

Using a passively stable attosecond beamline for relative photoemission time delays at high XUV photon energies

et al. 2018

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We present and demonstrate an experimental scheme that enables overlap-free reconstruction of attosecond beating by the interference of two-photon transition (RABBITT) measurements at high extreme-ultraviolet (XUV) photon energies. A compact passively-stabilized attosecond beamline employing a multilayer (ML) mirror allows us to obtain XUV pulses consisting of only two odd high-harmonic orders from an attosecond pulse train (APT). We compare our new technique to existing schemes that are used to perform RABBITT measurements and discuss how our scheme resolves the limitations imposed by spectral complexity of the harmonic comb at high photon energies. We further demonstrate first applications of our scheme for rare gases and gas mixtures, and show that this scheme can be extended to gas-molecule mixtures.

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“…Attosecond pulses produced by high-order harmonic generation in gases 13,14 enable measuring ultrafast electron dynamics, as shown in a series of seminal experiments [15][16][17][18][19][20][21][22] . Temporal information is obtained by pump/probe techniques combining attosecond pulses and a synchronized laser field.…”

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Attosecond electron–spin dynamics in Xe 4d photoionization

et al. 2020

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The photoionization of xenon atoms in the 70–100 eV range reveals several fascinating physical phenomena such as a giant resonance induced by the dynamic rearrangement of the electron cloud after photon absorption, an anomalous branching ratio between intermediate Xe+ states separated by the spin-orbit interaction and multiple Auger decay processes. These phenomena have been studied in the past, using in particular synchrotron radiation, but without access to real-time dynamics. Here, we study the dynamics of Xe 4d photoionization on its natural time scale combining attosecond interferometry and coincidence spectroscopy. A time-frequency analysis of the involved transitions allows us to identify two interfering ionization mechanisms: the broad giant dipole resonance with a fast decay time less than 50 as, and a narrow resonance at threshold induced by spin-flip transitions, with much longer decay times of several hundred as. Our results provide insight into the complex electron-spin dynamics of photo-induced phenomena.

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Orientation-dependent stereo Wigner time delay and electron localization in a small molecule

Abstract: We present orientation-dependent stereo Wigner time delays of CO molecules, which reveal the electron localization at the ionization moment. Together with theoretical calculations this constitutes a spatially-and temporally-resolved reconstruction of the molecular photoelectric effect.

Cited by 30 publications

References 12 publications

Attosecond timing of electron emission from a molecular shape resonance

Attosecond timing of electron emission from a molecular shape resonance

Using a passively stable attosecond beamline for relative photoemission time delays at high XUV photon energies

Attosecond electron–spin dynamics in Xe 4d photoionization

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