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  • Letter
  • Open Access

Emergence of resonating valence-bond correlations in stretched graphene

S. Azadi1,*, A. Principi1, T. D. Kühne2,3,4, and M. S. Bahramy1

  • *Contact author: sam.azadi@manchester.ac.uk

Phys. Rev. B 114, L111110 – Published 24 August, 2026

DOI: https://doi.org/10.1103/96cl-xq62

Abstract

Electronic correlations in graphene are generally considered weak due to the large bandwidth of its π electrons. Here we show that tensile expansion of the honeycomb lattice provides a direct route to enhancing correlation effects. Using variational and diffusion quantum Monte Carlo, we compare a conventional Jastrow-Slater determinant wave function with a resonating-valence-bond (RVB) Jastrow-antisymmetrized geminal product ansatz for a series of stretched graphene lattices. We find that the energy gain of the RVB state relative to the single-determinant description increases with bond expansion up to a critical strain δcr, and decreases beyond it, revealing a nonmonotonic evolution of electronic correlations. A quantitative analysis places δcr≈14–19% across the system sizes studied, extrapolating to 13.7±0.8% in the thermodynamic limit. Analysis of the optimized many-body pairing amplitude further reveals that this crossover is accompanied by a sharp, specific enhancement of π-orbital character in the nearest-neighbor pairing between adjacent carbon atoms, providing direct microscopic evidence for the emergence of RVB-like bonding. This behavior indicates a transition from a weakly correlated Dirac semimetal to a regime with enhanced nondynamic correlation and short-range singlet pairing. Our results provide direct many-body evidence that lattice expansion drives graphene into a regime where RVB-like correlations become energetically favorable, offering a simple route to tuning correlation effects in Dirac materials.

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