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Peng B, Lestrange PJ, Goings JJ, et al. Energy-Specific Equation-of-Motion Coupled-Cluster Methods for High-Energy Excited States: Application to K-edge X-ray Absorption Spectroscopy. J Chem Theory Comput. 2015;11(9):4146-53doi: 10.1021/acs.jctc.5b00459.
Peng, B., Lestrange, P. J., Goings, J. J., Caricato, M., & Li, X. (2015). Energy-Specific Equation-of-Motion Coupled-Cluster Methods for High-Energy Excited States: Application to K-edge X-ray Absorption Spectroscopy. Journal of chemical theory and computation, 11(9), 4146-53. https://doi.org/10.1021/acs.jctc.5b00459
Peng, Bo, et al. "Energy-Specific Equation-of-Motion Coupled-Cluster Methods for High-Energy Excited States: Application to K-edge X-ray Absorption Spectroscopy." Journal of chemical theory and computation vol. 11,9 (2015): 4146-53. doi: https://doi.org/10.1021/acs.jctc.5b00459
Peng B, Lestrange PJ, Goings JJ, Caricato M, Li X. Energy-Specific Equation-of-Motion Coupled-Cluster Methods for High-Energy Excited States: Application to K-edge X-ray Absorption Spectroscopy. J Chem Theory Comput. 2015 Sep 08;11(9):4146-53. doi: 10.1021/acs.jctc.5b00459. Epub 2015 Aug 13. PMID: 26575909.
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J Chem Theory Comput. 2015 Sep 08;11(9):4146-53. doi: 10.1021/acs.jctc.5b00459. Epub 2015 Aug 13.

Energy-Specific Equation-of-Motion Coupled-Cluster Methods for High-Energy Excited States: Application to K-edge X-ray Absorption Spectroscopy.

Journal of chemical theory and computation

Bo Peng, Patrick J Lestrange, Joshua J Goings, Marco Caricato, Xiaosong Li

Affiliations

  1. Department of Chemistry, University of Washington , Seattle, Washington 98195, United States.
  2. Department of Chemistry, University of Kansas , Lawrence, Kansas 66045, United States.

PMID: 26575909 DOI: 10.1021/acs.jctc.5b00459

Abstract

Single-reference techniques based on coupled-cluster (CC) theory, in the forms of linear response (LR) or equation of motion (EOM), are highly accurate and widely used approaches for modeling valence absorption spectra. Unfortunately, these equations with singles and doubles (LR-CCSD and EOM-CCSD) scale as O(N⁶), which may be prohibitively expensive for the study of high-energy excited states using a conventional eigensolver. In this paper, we present an energy-specific non-Hermitian eigensolver that is able to obtain high-energy excited states (e.g., XAS K-edge spectrum) at low computational cost. In addition, we also introduce an improved trial vector for iteratively solving the EOM-CCSD equation with a focus on high-energy eigenstates. The energy-specific EOM-CCSD approach and its low-scaling alternatives are applied to calculations of carbon, nitrogen, oxygen, and sulfur K-edge excitations. The results are compared to other implementations of CCSD for excited states, energy-specific linear response time-dependent density functional theory (TDDFT), and experimental results with multiple statistical metrics are presented and evaluated.

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