Data from: Linear scaling calculations of excitation energies with active-space particle-particle random phase approximation

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  • We developed an efficient active-space particle-particle random phase approximation (ppRPA) approach to calculate accurate charge-neutral excitation energies of molecular systems. The active-space ppRPA approach constrains both indexes in particle and hole pairs in the ppRPA matrix, which only selects frontier orbitals with dominant contributions to low-lying excitation energies. It employs truncation in both orbital indexes in the particle-particle and the hole-hole space. The resulting matrix, the eigenvalues of which are excitation energies, has a dimension that is independent of the size of the systems. The computational effort for the excitation energy calculation, therefore, scales linearly with system size, beyond the ground state calculation of (N-2)-electron system, where N is the electron number of the molecule. With the active space consisting of 30 occupied and 30 virtual orbitals, the active-space ppRPA approach predicts excitation energies of valence, charge-transfer, Rydberg, double and diradical excitations with the mean absolute errors (MAEs) smaller than 0.03 eV compared with the full-space ppRPA results. As a side product, we also applied the active-space ppRPA approach in the renormalized singles (RS) T-matrix approach. Combining the non-interacting pair approximation that approximates the contribution to the self-energy outside the active space, the active-space GRSTRS@PBE approach predicts accurate absolute and relative core-level binding energies with the MAE around 1.58 eV and 0.3 eV, respectively. The developed linear scaling calculation of excitation energies is promising for applications to large and complex systems. ... [Read More]

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8 files (137 MB)
Data Citation
  • Li, J., Yu, J., Zehua, C., & Yang, W. (2023). Data from: Linear scaling calculations of excitation energies with active-space particle-particle random phase approximation. Duke Research Data Repository. https://doi.org/10.7924/r4wm1g15c
DOI
  • 10.7924/r4wm1g15c
Publication Date
ARK
  • ark:/87924/r4wm1g15c
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Related Materials
  • Li, J., Yu, J., Chen, Z., & Yang, W. (2023). Linear scaling calculations of excitation energies with active-space Particle–Particle random-phase approximation. The Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, & General Theory, 127(37), 7811-7822.  https://doi.org/10.1021/acs.jpca.3c02834
Funding Agency
  • National Science Foundation
  • National Institutes of Health
Grant Number
  • CHE-2154831
  • R01-GM061870
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  • Data from: Linear scaling calculations of excitation energies with active-space particle-particle random phase approximation
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Thumbnail Title Date Uploaded Visibility Actions
file details README.md 2023-04-28 Public Download
file details core65_grstrs.zip 2023-04-28 Public Download
file details diradical_st_gap.zip 2023-04-28 Public Download
file details double_excitation.zip 2023-04-28 Public Download
file details hydrocarbon_st_gap.zip 2023-04-28 Public Download
file details rydberg_excitation.zip 2023-04-28 Public Download
file details stein_ct_set.zip 2023-04-28 Public Download
file details thiel_set.zip 2023-04-28 Public Download

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