English

Sixteen-State Energy Mapping for First-Principles Four-Spin Ring Exchange: Validation on $La_2CuO_4$ and $SrFeO_2$

Materials Science 2026-07-21 v1 Strongly Correlated Electrons Quantum Physics

Abstract

Four-spin ring (cyclic) exchange JringJ_{ring} is an essential ingredient of the Heisenberg spin Hamiltonian of cuprates and other square-lattice magnets, yet it has lacked the kind of direct, local first-principles extraction that the four-state method provides for bilinear exchange, JJ. We supply it by generalizing that method to a sixteen-state (242^4) scheme. Symmetry reduces the sixteen configurations to six or eight inequivalent energies, so the cost is modest. The derivation also shows that the conventional four-state magnetic coupling, JJ, is itself ring-renormalized, by ±2JringS2\pm 2 J_{ring} S^2 with the sign set by the reference state. T-La2_2CuO4_4 confirms this quantitatively: three independent routes agree on JringJ_{ring} to 0.2%0.2\%, giving Jring/J1=0.25J_{ring}/J_1 = 0.25, and a four-state J1J_1 quoted without naming its reference is wrong by 12%12\% in this material. The direct sixteen-state extraction itself proves reference-dependent, the N\'eel and ferromagnetic baths bracketing the mapping value: a fourth-order fingerprint of interactions beyond the pair-plus-ring model, which additional reference baths resolve into a bare JringJ_{ring} and a converging tower of six- and eight-spin loop couplings. SrFeO2_2 (S=2S = 2), with the same plaquette yet Jring/J=0.006J_{ring}/J = 0.006, provides the negative control: a plaquette is necessary for ring exchange, far from sufficient. The complete workflow, including the band-gap and local-moment diagnostics that certify any such extraction, is implemented in the openly available Mag4 package, so that JringJ_{ring} costs no more effort to obtain than JJ.

Keywords

Cite

@article{arxiv.2607.18986,
  title  = {Sixteen-State Energy Mapping for First-Principles Four-Spin Ring Exchange: Validation on $La_2CuO_4$ and $SrFeO_2$},
  author = {Xavier Rocquefelte and Peter Blaha},
  journal= {arXiv preprint arXiv:2607.18986},
  year   = {2026}
}

Comments

37 pages, 4 figures, 6 Tables