Hybrid Quantum-Classical Simulations of Graphene Analogues: Adsorption Energetics Beyond DFT

Understanding strongly correlated systems is essential for advancing quantum chemistry and materials science, yet conventional methods like Density Functional Theory (DFT) often fail to capture their complex electronic behavior. To address these limitations, we develop a hybrid quantum-classical framework that integrates Multiconfigurational Self-Consistent Field (MCSCF) with the Variational Quantum Eigensolver (VQE). Our initial benchmarks on water dissociation enabled the systematic optimization of key computational parameters, including ansatz selection, active space construction, and error mitigation. Building on this, we extend our approach to investigate the interactions between graphene analogues and water, demonstrating that our framework produces binding energies consistent with high-accuracy quantum methods. Furthermore, we apply this methodology to predict the binding energies of transition metals (Fe, Co, Ni) on both pristine and defective graphene analogues, revealing strong charge transfer effects and pronounced multireference character─phenomena often misrepresented by standard DFT. In contrast to many existing quantum algorithms that are constrained to small molecular systems, our framework achieves chemically accurate predictions for larger, strongly correlated systems such as metal-graphene complexes. This advancement highlights the capacity of hybrid quantum-classical approaches to address complex electronic interactions and demonstrates a practical route toward realizing quantum advantage for real-world materials applications in the Noisy Intermediate-Scale Quantum (NISQ) era.

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Publication Details

Journal
The Journal of Physical Chemistry A
Published
2026-01-13
DOI
https://doi.org/10.1021/acs.jpca.5c06607
Primary Topic
Machine Learning in Materials Science
Type
article
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article

Hybrid Quantum-Classical Simulations of Graphene Analogues: Adsorption Energetics Beyond DFT

Archith Rayabharam, N. R. Aluru
The Journal of Physical Chemistry A
Machine Learning in Materials Science
article

Hybrid Quantum-Classical Simulations of Graphene Analogues: Adsorption Energetics Beyond DFT

Archith Rayabharam, N. R. Aluru
article en

Abstract

Understanding strongly correlated systems is essential for advancing quantum chemistry and materials science, yet conventional methods like Density Functional Theory (DFT) often fail to capture their complex electronic behavior. To address these limitations, we develop a hybrid quantum-classical framework that integrates Multiconfigurational Self-Consistent Field (MCSCF) with the Variational Quantum Eigensolver (VQE). Our initial benchmarks on water dissociation enabled the systematic optimization of key computational parameters, including ansatz selection, active space construction, and error mitigation. Building on this, we extend our approach to investigate the interactions between graphene analogues and water, demonstrating that our framework produces binding energies consistent with high-accuracy quantum methods. Furthermore, we apply this methodology to predict the binding energies of transition metals (Fe, Co, Ni) on both pristine and defective graphene analogues, revealing strong charge transfer effects and pronounced multireference character─phenomena often misrepresented by standard DFT. In contrast to many existing quantum algorithms that are constrained to small molecular systems, our framework achieves chemically accurate predictions for larger, strongly correlated systems such as metal-graphene complexes. This advancement highlights the capacity of hybrid quantum-classical approaches to address complex electronic interactions and demonstrates a practical route toward realizing quantum advantage for real-world materials applications in the Noisy Intermediate-Scale Quantum (NISQ) era.

The Journal of Physical Chemistry AVol. 130(4)
Walker (United States) (US), The University of Texas at Austin (US)
Openalex Percentile: Top 89%
Machine Learning in Materials Science
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Hybrid Quantum-Classical Simulations of Graphene Analogues: Adsorption Energetics Beyond DFT — Archith Rayabharam, N. R. Aluru · The Journal of Physical Chemistry A (2026) | TGRS Research Map | TGRS