Probing molecular environment through photoemission delays

Biswas, S.; Förg, Benjamin; Ortmann, Lisa; Schötz, Johannes; Schweinberger, Wolfgang; Zimmermann, Tomáš; Pi, Liang-Wen; Baykusheva, Denitsa; Masood, Hafiz; Liontos, I.; Kamal, A. M.; Kling, Nora G.; Alharbi, Abdullah; Alharbi, Meshaal; Azzeer, Abdallah M.; Hartmann, Gregor; Wörner, Hans Jakob; Landsman, Alexandra S.; Kling, Matthias F.

doi:10.1038/s41567-020-0887-8

Cited by 60 publications

(42 citation statements)

References 43 publications

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“…Our experimental approach, which adds temporal information to traditional spectral studies, provides increased understanding of the complex electron dynamics taking place in Xe 4 d photoionization. Finally, shape resonances are ubiquitous in nature and the methods developed in this work should be useful to investigate the electronic properties of a variety of molecular systems (see recent work in N 2 42 and CH 3 I 43 ).…”

Section: Discussionmentioning

confidence: 99%

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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Section: Discussionmentioning

confidence: 99%

Attosecond electron–spin dynamics in Xe 4d photoionization

et al. 2020

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“…In this work, we applied attosecond spectroscopy to study liquid water. Whereas isolated molecules of increasing complexity have been studied with attosecond temporal resolution (14)(15)(16)(17), a deeper understanding of electronic dynamics in real chemical and biological processes requires an extension of attosecond science to the liquid phase. As the main distinguishing feature compared to most femtosecond spectroscopies, the inherent time scale of the present measurements freezes all types of structural dynamics, leaving only the fastest electronic dynamics as possible contributions.…”

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confidence: 99%

Attosecond spectroscopy of liquid water

Jordan

Huppert

Rattenbacher

et al. 2020

Science

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Electronic dynamics in liquids are of fundamental importance, but time-resolved experiments have so far remained limited to the femtosecond time scale. We report the extension of attosecond spectroscopy to the liquid phase. We measured time delays of 50 to 70 attoseconds between the photoemission from liquid water and that from gaseous water at photon energies of 21.7 to 31.0 electron volts. These photoemission delays can be decomposed into a photoionization delay sensitive to the local environment and a delay originating from electron transport. In our experiments, the latter contribution is shown to be negligible. By referencing liquid water to gaseous water, we isolated the effect of solvation on the attosecond photoionization dynamics of water molecules. Our methods define an approach to separating bound and unbound electron dynamics from the structural response of the solvent.

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“…This subject is of great interest for the formation of photoemission delays in attosecond science or for the molecular imaging in optical field emission with intense laser pulses. 15,16,[65][66][67][68] The paper is organized as follows. Next section presents the methodology: TDSE solution under the WPP scheme, strategy to construct the potential of the active electron, and how to extract the relevant information from the propagation.…”

Section: Introductionmentioning

confidence: 99%

Ultrafast Dynamics of Electronic Resonances in Molecules Adsorbed on Metal Surfaces: A Wave Packet Propagation Approach

Aguilar-Galindo

Borisov

Díaz‐Tendero

2021

J. Chem. Theory Comput.

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We present a wave packet propagation-based method to study the electron dynamics in molecular species in the gas phase and adsorbed on metal surfaces. It is a very general method that can be employed to any system where the electron dynamics is dominated by an active electron and the coupling between the discrete and continuum electronic states is of importance. As an example one can consider resonant moleculesurface electron transfer or molecular photoionization. Our approach is based on a 1 computational strategy allowing to incorporate ab initio inputs from Quantum Chemistry methods, such as Density Functional Theory, Hartree-Fock and Coupled Cluster.Thus, the electronic structure of the molecule is fully taken into account. The electron wave function is represented on a 3D grid in spatial coordinates, and its temporal evolution is obtained from the solution of the time dependent Schrödinger equation. We illustrate our method with an example -electron dynamics of anionic states localized on organic molecules adsorbed on metal surfaces. In particular, we study resonant charge transfer from π * orbitals of three vinyl derivatives (acrylamide, acrylonitrile, and acrolein) adsorbed on a Cu(100) surface. Electron transfer between these lowest unoccupied molecular orbitals and the metal surface is extremely fast, leading to a decay of the population of the molecular anion on the femtosecond timescale. We detail how to analyze the time-dependent electronic wave function in order to obtain the relevant information on the system: the energies and lifetimes of the molecule-localized quasi-stationary states, their associated resonant wavefunctions, and the population decay channels. In particular, we demonstrate the effect of the electronic structure of the substrate on the energy and wave vector distribution of the hot electrons injected into the metal by the decaying molecular resonance.

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Probing molecular environment through photoemission delays

Cited by 60 publications

References 43 publications

Attosecond electron–spin dynamics in Xe 4d photoionization

Attosecond electron–spin dynamics in Xe 4d photoionization

Attosecond spectroscopy of liquid water

Ultrafast Dynamics of Electronic Resonances in Molecules Adsorbed on Metal Surfaces: A Wave Packet Propagation Approach

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