Revealing the role of electron-electron correlations by mapping dissociation of highly excited using ultrashort XUV pulses
- Univ. of Colorado and NIST, Boulder, CO (United States)
- Univ. Autonoma de Madrid, Madrid (Spain)
- Univ. of Tsukuba, Ibaraki (Japan)
- Univ. de Antioquia, Medellin (Colombia)
- Univ. Frankfurt, Frankfurt (Germany)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Univ. Autonoma de Madrid, Madrid (Spain); Instituto Madrileno de Estudios Avanzados en Nanociencia (IMDEA Nano), Madrid (Spain); Univ. Autonoma de Madrid, Madrid (Spain)
- Univ. of Colorado and NIST, Boulder, CO (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); ETH Zurich, Zurich (Switzerland)
Understanding electron-electron correlations in matter ranging from atoms to solids represents a grand challenge for both experiment and theory. Here, these correlations occur on attosecond timescales and have only recently become experimentally accessible. In the case of highly excited systems, the task of understanding and probing correlated interactions is even greater. In this work, we combine state-of-the-art light sources and advanced detection techniques with ab initio calculations to unravel the role of electron-electron correlation in photoionization by mapping the dissociation of a highly excited molecule. Correlations between the two electrons dictate the pathways along which the molecule dissociates and lead to a superposition of excited ionic states. Using 3D Coulomb explosion imaging and electron-ion coincidence techniques, we assess the relative contribution of competing parent ion states to the dissociation process for different orientations of the molecule with respect to the laser polarization, which is consistent with a shake-up ionization process. As a step toward observing coherent superposition experimentally, we map the relevant nuclear potentials using Coulomb explosion imaging and show theoretically that such an experiment could confirm this coherence via two-path interference.
- Research Organization:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of Colorado, Boulder, CO (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES), Chemical Sciences, Geosciences & Biosciences Division
- Grant/Contract Number:
- AC02-05CH11231; FG02-99ER14982
- OSTI ID:
- 1461171
- Alternate ID(s):
- OSTI ID: 1455099; OSTI ID: 1686147; OSTI ID: 1686150; OSTI ID: 1907881
- Journal Information:
- Physical Review A, Vol. 97, Issue 6; Related Information: © 2018 American Physical Society.; ISSN 2469-9926
- Publisher:
- American Physical Society (APS)Copyright Statement
- Country of Publication:
- United States
- Language:
- English
Web of Science
The quantum chemistry of attosecond molecular science
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journal | July 2019 |
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