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Area of Science:

  • Computational Chemistry
  • Quantum Chemistry
  • Electronic Structure Theory

Background:

  • Selected configuration interaction (SCI) methods offer advantages over full CI but still exhibit exponential computational scaling.
  • Inaccuracies in describing electron correlation at short distances slow down energy convergence with basis set size.

Purpose of the Study:

  • To investigate the efficacy of non-Hermitian, transcorrelated (TC) SCI for improving computational efficiency and accuracy.
  • To assess the impact of TC-SCI on determinant space size and energy convergence rates.
  • To explore the relationship between correlation factor accuracy and TC-SCI performance.

Main Methods:

  • Application of non-Hermitian, transcorrelated (TC) selected configuration interaction (SCI) algorithms.
  • Systematic investigation using small molecular systems.
  • Utilizing increasingly large one-electron basis sets.

Main Results:

  • TC-SCI significantly compacts the determinant space compared to conventional SCI.
  • Achieves desired accuracy with a reduced number of determinants.
  • Demonstrates accelerated convergence of electronic energy with increasing basis set size.

Conclusions:

  • TC-SCI offers a computationally efficient and accurate approach for electronic structure calculations.
  • The accuracy of the correlation factor is crucial for the observed improvements in determinant space compression and energy convergence.
  • TC-SCI shows promise for tackling larger and more complex quantum chemistry problems.