Strong-field ionization of complex molecules

Strong-field photoelectron momentum imaging of the prototypical biomolecule indole is disentangled in a combined experimental and computational approach. Experimentally, strong control over the molecules enables the acquisition of photoelectron momentum distributions in the molecular frame for a wel...

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Main Authors: Joss Wiese, Jolijn Onvlee, Sebastian Trippel, Jochen Küpper
Format: Article
Language:English
Published: American Physical Society 2021-01-01
Series:Physical Review Research
Online Access:http://doi.org/10.1103/PhysRevResearch.3.013089
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author Joss Wiese
Jolijn Onvlee
Sebastian Trippel
Jochen Küpper
author_facet Joss Wiese
Jolijn Onvlee
Sebastian Trippel
Jochen Küpper
author_sort Joss Wiese
collection DOAJ
description Strong-field photoelectron momentum imaging of the prototypical biomolecule indole is disentangled in a combined experimental and computational approach. Experimentally, strong control over the molecules enables the acquisition of photoelectron momentum distributions in the molecular frame for a well-defined narrow range of incident intensities. A highly efficient semiclassical simulation setup based on the adiabatic tunneling theory quantitatively reproduces these results. Jointly, experiment and computations reveal holographic structures in the asymptotic momentum distributions, which are found to sensitively depend on the alignment of the molecular frame. We identify the essential molecular properties that shape the photoelectron wave packet in the first step of the ionization process and employ a quantum-chemically exact description of the cation during the subsequent continuum dynamics. The detailed modeling of the molecular ion, which accounts for its polarization by the laser electric field, enables the accurate description of the photoelectron dynamics in close vicinity of the molecule. Our approach provides full insight into the photoelectron's dynamics in terms of semiclassical trajectories and aims at the simulation and unraveling of strong-field diffractive imaging of biomolecular systems on femtosecond timescales.
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spelling doaj.art-694028e47b3e4e1caf33a6888b9a8bd32024-04-12T17:06:45ZengAmerican Physical SocietyPhysical Review Research2643-15642021-01-013101308910.1103/PhysRevResearch.3.013089Strong-field ionization of complex moleculesJoss WieseJolijn OnvleeSebastian TrippelJochen KüpperStrong-field photoelectron momentum imaging of the prototypical biomolecule indole is disentangled in a combined experimental and computational approach. Experimentally, strong control over the molecules enables the acquisition of photoelectron momentum distributions in the molecular frame for a well-defined narrow range of incident intensities. A highly efficient semiclassical simulation setup based on the adiabatic tunneling theory quantitatively reproduces these results. Jointly, experiment and computations reveal holographic structures in the asymptotic momentum distributions, which are found to sensitively depend on the alignment of the molecular frame. We identify the essential molecular properties that shape the photoelectron wave packet in the first step of the ionization process and employ a quantum-chemically exact description of the cation during the subsequent continuum dynamics. The detailed modeling of the molecular ion, which accounts for its polarization by the laser electric field, enables the accurate description of the photoelectron dynamics in close vicinity of the molecule. Our approach provides full insight into the photoelectron's dynamics in terms of semiclassical trajectories and aims at the simulation and unraveling of strong-field diffractive imaging of biomolecular systems on femtosecond timescales.http://doi.org/10.1103/PhysRevResearch.3.013089
spellingShingle Joss Wiese
Jolijn Onvlee
Sebastian Trippel
Jochen Küpper
Strong-field ionization of complex molecules
Physical Review Research
title Strong-field ionization of complex molecules
title_full Strong-field ionization of complex molecules
title_fullStr Strong-field ionization of complex molecules
title_full_unstemmed Strong-field ionization of complex molecules
title_short Strong-field ionization of complex molecules
title_sort strong field ionization of complex molecules
url http://doi.org/10.1103/PhysRevResearch.3.013089
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AT jolijnonvlee strongfieldionizationofcomplexmolecules
AT sebastiantrippel strongfieldionizationofcomplexmolecules
AT jochenkupper strongfieldionizationofcomplexmolecules