Attosecond Photoionization Dynamics: from Molecules over Clusters to the Liquid Phase

Photoionization is a process taking place on attosecond time scales. How its properties evolve from isolated particles to the condensed phase is an open question of both fundamental and practical relevance. Here, we review recent work that has advanced the study of photoionization dynamics from ato...

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Main Authors: Xiaochun Gong, Inga Jordan, Martin Huppert, Saijoscha Heck, Denitsa Baykusheva, Denis Jelovina, Axel Schild, Hans Jakob Wörner
Format: Article
Language:deu
Published: Swiss Chemical Society 2022-06-01
Series:CHIMIA
Subjects:
Online Access:https://chimia.ch/chimia/article/view/6063
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author Xiaochun Gong
Inga Jordan
Martin Huppert
Saijoscha Heck
Denitsa Baykusheva
Denis Jelovina
Axel Schild
Hans Jakob Wörner
author_facet Xiaochun Gong
Inga Jordan
Martin Huppert
Saijoscha Heck
Denitsa Baykusheva
Denis Jelovina
Axel Schild
Hans Jakob Wörner
author_sort Xiaochun Gong
collection DOAJ
description Photoionization is a process taking place on attosecond time scales. How its properties evolve from isolated particles to the condensed phase is an open question of both fundamental and practical relevance. Here, we review recent work that has advanced the study of photoionization dynamics from atoms to molecules, clusters and the liquid phase. The first measurements of molecular photoionization delays have revealed the attosecond dynamics of electron emission from a molecular shape resonance and their sensitivity to the molecular potential. Using electron-ion coincidence spectroscopy these measurements have been extended from isolated molecules to clusters. A continuous increase of the delays with the water-cluster size has been observed up to a size of 4-5 molecules, followed by a saturation towards larger clusters. Comparison with calculations has revealed a correlation of the time delay with the spatial extension of the created electron hole. Using cylindrical liquid-microjet techniques, these measurements have also been extended to liquid water, revealing a delay relative to isolated water molecules that was very similar to the largest water clusters studied. Detailed modeling based on Monte-Carlo simulations confirmed that these delays are dominated by the contributions of the first two solvation shells, which agrees with the results of the cluster measurements. These combined results open the perspective of experimentally characterizing the delocalization of electronic wave functions in complex systems and studying their evolution on attosecond time scales.
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spelling doaj.art-722acdacc52744ae925c4c76e2ccaa262022-12-22T02:47:43ZdeuSwiss Chemical SocietyCHIMIA0009-42932673-24242022-06-0176610.2533/chimia.2022.520Attosecond Photoionization Dynamics: from Molecules over Clusters to the Liquid PhaseXiaochun Gong0Inga Jordan1Martin Huppert2Saijoscha Heck3Denitsa Baykusheva4Denis Jelovina5Axel Schild6Hans Jakob Wörner7State Key laboratory of precision spectroscopy, East China Normal University, 500 Dongchuan Road, Shanghai, ChinaLaboratorium für Physikalische Chemie, ETH Zürich, CH-8093 ZürichPaul Scherrer Institute, Forschungsstrasse 111, 5232 Villigen PSILaboratorium für Physikalische Chemie, ETH Zürich, CH-8093 ZürichDepartment of Physics, Harvard University 17, Oxford Street, Cambridge, MA 02138Laboratorium für Physikalische Chemie, ETH Zürich, CH-8093 ZürichLaboratorium für Physikalische Chemie, ETH Zürich, CH-8093 ZürichLaboratorium für Physikalische Chemie, ETH Zürich, CH-8093 Zürich Photoionization is a process taking place on attosecond time scales. How its properties evolve from isolated particles to the condensed phase is an open question of both fundamental and practical relevance. Here, we review recent work that has advanced the study of photoionization dynamics from atoms to molecules, clusters and the liquid phase. The first measurements of molecular photoionization delays have revealed the attosecond dynamics of electron emission from a molecular shape resonance and their sensitivity to the molecular potential. Using electron-ion coincidence spectroscopy these measurements have been extended from isolated molecules to clusters. A continuous increase of the delays with the water-cluster size has been observed up to a size of 4-5 molecules, followed by a saturation towards larger clusters. Comparison with calculations has revealed a correlation of the time delay with the spatial extension of the created electron hole. Using cylindrical liquid-microjet techniques, these measurements have also been extended to liquid water, revealing a delay relative to isolated water molecules that was very similar to the largest water clusters studied. Detailed modeling based on Monte-Carlo simulations confirmed that these delays are dominated by the contributions of the first two solvation shells, which agrees with the results of the cluster measurements. These combined results open the perspective of experimentally characterizing the delocalization of electronic wave functions in complex systems and studying their evolution on attosecond time scales. https://chimia.ch/chimia/article/view/6063attosecond spectroscopyphotoionization delaysmolecular photoionizationwater clustersliquid waterelectron scattering
spellingShingle Xiaochun Gong
Inga Jordan
Martin Huppert
Saijoscha Heck
Denitsa Baykusheva
Denis Jelovina
Axel Schild
Hans Jakob Wörner
Attosecond Photoionization Dynamics: from Molecules over Clusters to the Liquid Phase
CHIMIA
attosecond spectroscopy
photoionization delays
molecular photoionization
water clusters
liquid water
electron scattering
title Attosecond Photoionization Dynamics: from Molecules over Clusters to the Liquid Phase
title_full Attosecond Photoionization Dynamics: from Molecules over Clusters to the Liquid Phase
title_fullStr Attosecond Photoionization Dynamics: from Molecules over Clusters to the Liquid Phase
title_full_unstemmed Attosecond Photoionization Dynamics: from Molecules over Clusters to the Liquid Phase
title_short Attosecond Photoionization Dynamics: from Molecules over Clusters to the Liquid Phase
title_sort attosecond photoionization dynamics from molecules over clusters to the liquid phase
topic attosecond spectroscopy
photoionization delays
molecular photoionization
water clusters
liquid water
electron scattering
url https://chimia.ch/chimia/article/view/6063
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AT saijoschaheck attosecondphotoionizationdynamicsfrommoleculesoverclusterstotheliquidphase
AT denitsabaykusheva attosecondphotoionizationdynamicsfrommoleculesoverclusterstotheliquidphase
AT denisjelovina attosecondphotoionizationdynamicsfrommoleculesoverclusterstotheliquidphase
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