Title: Revealing the role of electron-electron correlations by mapping dissociation of highly excited ${{\mathrm{D}}_2}^{+}$ using ultrashort XUV pulses

Abstract

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 ${{\mathrm{D}}_2}^{}$ photoionization by mapping the dissociation of a highly excited ${{\mathrm{D}}_2}^{+}$ 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.

Authors:

Martin, L. ^[1]; Bello, R. Y. ^[2]; Hogle, C. W. ^[1]; Palacios, Alicia ^[2]; Tong, X. M. ^[3]; Sanz-Vicario, J. L. ^[4]; Jahnke, T. ^[5]; Schoffler, M. ^[5]; Dorner, R. ^[5]; Weber, Th. ^[6]; Martin, F. ^[7]; Kapteyn, H. C. ^[1]; Murnane, M. M. ^[1]; Ranitovic, P. ^[8]

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+ Show Author Affiliations

1. Univ. of Colorado and NIST, Boulder, CO (United States)
2. Univ. Autonoma de Madrid, Madrid (Spain)
3. Univ. of Tsukuba, Ibaraki (Japan)
4. Univ. de Antioquia, Medellin (Colombia)
5. Univ. Frankfurt, Frankfurt (Germany)
6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
7. Univ. Autonoma de Madrid, Madrid (Spain); Instituto Madrileno de Estudios Avanzados en Nanociencia (IMDEA Nano), Madrid (Spain); Univ. Autonoma de Madrid, Madrid (Spain)
8. Univ. of Colorado and NIST, Boulder, CO (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); ETH Zurich, Zurich (Switzerland)

Publication Date:

Wed Jun 20 00:00:00 EDT 2018

Research Org.:

Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of Colorado, Boulder, CO (United States)

Sponsoring Org.:

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

OSTI Identifier:

1461171

Alternate Identifier(s):

OSTI ID: 1455099; OSTI ID: 1686147; OSTI ID: 1686150; OSTI ID: 1907881

Grant/Contract Number:  

AC02-05CH11231; FG02-99ER14982

Resource Type:

Accepted Manuscript

Journal Name:

Physical Review A

Additional Journal Information:

Journal Volume: 97; Journal Issue: 6; Related Information: © 2018 American Physical Society.; Journal ID: ISSN 2469-9926

Publisher:

American Physical Society (APS)

Country of Publication:

United States

Language:

English

Subject:

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS; 74 ATOMIC AND MOLECULAR PHYSICS; Electron correlation calculations for atoms & ions; High-order harmonic generation; Laser dynamics; Quantum description of light-matter interaction; Ultrafast phenomena