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Title: A theoretical and experimental benchmark study of core-excited states in nitrogen

Abstract

The high resolution near edge X-ray absorption fine structure spectrum of nitrogen displays the vibrational structure of the core-excited states. This makes nitrogen well suited for assessing the accuracy of different electronic structure methods for core excitations. We report high resolution experimental measurements performed at the SOLEIL synchrotron facility. These are compared with theoretical spectra calculated using coupled cluster theory and algebraic diagrammatic construction theory. The coupled cluster singles and doubles with perturbative triples model known as CC3 is shown to accurately reproduce the experimental excitation energies as well as the spacing of the vibrational transitions. In conclusion, the computational results are also shown to be systematically improved within the coupled cluster hierarchy, with the coupled cluster singles, doubles, triples, and quadruples method faithfully reproducing the experimental vibrational structure.

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [3];  [4]; ORCiD logo [5];  [6]; ORCiD logo [7]
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  1. Univ. of Oslo (Norway). Hylleraas Centre for Quantum Molecular Sciences, Dept. of Chemistry; Norwegian Univ. of Science and Technology, Trondheim (Norway). Dept. of Chemistry; SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); Stanford Univ., CA (United States). Dept. of Chemistry
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
  3. Johns Hopkins Univ., Baltimore, MD (United States). Department of Chemistry
  4. Synchrotron SOLEIL, Saint-Aubin, Gif-sur-Yvette Cedex (France); Lund Univ. (Sweden). Dept. of Physics
  5. Technical Univ. of Denmark, Lyngby (Denmark). Dept. of Chemistry; Aarhus Univ. (Denmark). Aarhus Inst. of Advanced Studies
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); Univ. of Potsdam, Potsdam (Germany). Dept. of Physics and Astronomy
  7. Norwegian Univ. of Science and Technology, Trondheim (Norway). Dept. of Chemistry; SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); Stanford Univ., CA (United States). Dept. of Chemistry
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Org.:
USDOE; German National Academy of Sciences Leopoldina
OSTI Identifier:
1427025
Grant/Contract Number:  
AC02-76SF00515; 639508; 609033
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 148; Journal Issue: 6; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Myhre, Rolf H., Wolf, Thomas J. A., Cheng, Lan, Nandi, Saikat, Coriani, Sonia, Gühr, Markus, and Koch, Henrik. A theoretical and experimental benchmark study of core-excited states in nitrogen. United States: N. p., 2018. Web. doi:10.1063/1.5011148.
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Myhre, Rolf H., Wolf, Thomas J. A., Cheng, Lan, Nandi, Saikat, Coriani, Sonia, Gühr, Markus, & Koch, Henrik. A theoretical and experimental benchmark study of core-excited states in nitrogen. United States. https://doi.org/10.1063/1.5011148
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Myhre, Rolf H., Wolf, Thomas J. A., Cheng, Lan, Nandi, Saikat, Coriani, Sonia, Gühr, Markus, and Koch, Henrik. Wed . "A theoretical and experimental benchmark study of core-excited states in nitrogen". United States. https://doi.org/10.1063/1.5011148. https://www.osti.gov/servlets/purl/1427025.
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@article{osti_1427025,
title = {A theoretical and experimental benchmark study of core-excited states in nitrogen},
author = {Myhre, Rolf H. and Wolf, Thomas J. A. and Cheng, Lan and Nandi, Saikat and Coriani, Sonia and Gühr, Markus and Koch, Henrik},
abstractNote = {The high resolution near edge X-ray absorption fine structure spectrum of nitrogen displays the vibrational structure of the core-excited states. This makes nitrogen well suited for assessing the accuracy of different electronic structure methods for core excitations. We report high resolution experimental measurements performed at the SOLEIL synchrotron facility. These are compared with theoretical spectra calculated using coupled cluster theory and algebraic diagrammatic construction theory. The coupled cluster singles and doubles with perturbative triples model known as CC3 is shown to accurately reproduce the experimental excitation energies as well as the spacing of the vibrational transitions. In conclusion, the computational results are also shown to be systematically improved within the coupled cluster hierarchy, with the coupled cluster singles, doubles, triples, and quadruples method faithfully reproducing the experimental vibrational structure.},
doi = {10.1063/1.5011148},
journal = {Journal of Chemical Physics},
number = 6,
volume = 148,
place = {United States},
year = {2018},
month = {2}
}
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https://doi.org/10.1063/1.5011148
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Cited by: 22 works
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Figures / Tables:

Figure 1 Figure 1: Comparison of CC3 and experiment for the four lowest excited states. The intensity of the first peak is normalized to 1 and empirical line broadening added to the theoretical spectrum.
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    Works referencing / citing this record:

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    Coupled cluster study of the x-ray absorption spectra of formaldehyde derivatives at the oxygen, carbon, and fluorine K-edges
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