Divergences in classical and quantum linear response and equation of motion formulations

Erik Rosendahl Kjellgren*, Peter Reinholdt, Karl Michael Ziems, Stephan P. A. Sauer, Sonia Coriani, Jacob Kongsted

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

2 Downloads (Pure)

Abstract

Calculating molecular properties using quantum devices can be done through the quantum linear response (qLR) or, equivalently, the quantum equation of motion (qEOM) formulations. Different parameterizations of qLR and qEOM are available, namely naive, projected, self-consistent, and state-transfer. In the naive and projected parameterizations, the metric is not the identity, and we show that it depends on the redundant orbital rotations. This dependency may lead to divergences in the excitation energies for certain choices of the redundant orbital rotation parameters in an idealized noise-less setting. Further, this leads to significant variance when calculations include statistical noise from finite quantum sampling.
Original languageEnglish
Article number124112
JournalThe Journal of Chemical Physics
Volume161
Issue number16
Number of pages8
ISSN0021-9606
DOIs
Publication statusPublished - 2024

Keywords

  • Faculty of Science
  • Qunatum Computing
  • linear response theory
  • excitation energies

Cite this