| Autor: |
Gaspard L; Laboratoire de Chimie et Physique Quantiques, Université Toulouse III─Paul Sabatier, Toulouse 31062, France., Martins C; Laboratoire de Chimie et Physique Quantiques, Université Toulouse III─Paul Sabatier, Toulouse 31062, France., Malrieu JP; Laboratoire de Chimie et Physique Quantiques, Université Toulouse III─Paul Sabatier, Toulouse 31062, France. |
| Jazyk: |
angličtina |
| Zdroj: |
The journal of physical chemistry. A [J Phys Chem A] 2024 Nov 28; Vol. 128 (47), pp. 10272-10281. Date of Electronic Publication: 2024 Nov 15. |
| DOI: |
10.1021/acs.jpca.4c04277 |
| Abstrakt: |
In quantum chemistry, single-reference Coupled Cluster theory, and its refinements introduced by Bartlett, has become a "gold-standard" predictive method for taking into account electronic correlations in molecules. In this article, we introduce a new formalism based on a Coupled Cluster expansion of the wave function that is suited to describe model periodic systems and apply this methodology to the case of hole-doped antiferromagnetic two-dimensional (2D)-square spin-lattices as a proof of concept. More precisely, we focus our study on 1/5 and 1/7 doping ratios and discuss the possible ordering effect due to large hole-hole repulsion. Starting from one of the equivalent single determinants exhibiting a full spin alternation and the most remote location of the holes as a single reference, the method incorporates some corrections to the traditional Coupled Cluster formalism to take into account the nonadditivity of excitation energies to multiply excited determinants. The amplitudes of the excitations, which are possible on the excited determinants but impossible on the reference, are evaluated perturbatively, while their effect is treated as a dressing in the basic equations. The expansion does not show any sign of divergence of the wave operator. Finally, the probabilities of holes moving toward the first- and second-neighboring sites are reported, which confirms the importance of the hole-hole repulsion and offers a picture of how stripes expand around its central line in the "stripe phases" observed in cuprates. |
| Databáze: |
MEDLINE |
| Externí odkaz: |
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