English

Excited states in variational Monte Carlo using a penalty method

Chemical Physics 2021-10-15 v2 Materials Science

Abstract

The authors present a technique using variational Monte Carlo to solve for excited states of electronic systems. The technique is based on enforcing orthogonality to lower energy states, which results in a simple variational principle for the excited states. Energy optimization is then used to solve for the excited states. This technique is applied to the well-characterized benzene molecule, in which \sim10,000 parameters are optimized for the first 12 excited states. Agreement within approximately 0.2 eV is obtained with higher scaling coupled cluster methods; small disagreements with experiment are likely due to vibrational effects.

Keywords

Cite

@article{arxiv.2009.13556,
  title  = {Excited states in variational Monte Carlo using a penalty method},
  author = {Shivesh Pathak and Brian Busemeyer and João N. B. Rodrigues and Lucas K. Wagner},
  journal= {arXiv preprint arXiv:2009.13556},
  year   = {2021}
}
R2 v1 2026-06-23T18:51:29.217Z