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<p>Many-body fermionic Diffusion Monte Carlo (DMC) methods are applied to accurately predict the fundamental gap of the monolayer ferromagnet CrI<sub>3</sub>. The fundamental gap obtained, Δ<sub><i>f</i></sub> = 2.9(1) eV, agrees well with the highest peak in optical spectroscopy measurements and a previous <i>G</i><i>W</i> result. We numerically show that the same value of Δ<sub><i>f</i></sub> is obtained in the thermodynamic limit using both neutral promotions and the standard definition of Δ<sub><i>f</i></sub> based on the ionization potential and electron affinity. Analysis of the differences between density matrices of natural orbitals obtained from configuration interaction calculations explains why a single-reference trial wave function can produce an accurate excitation. We find that accounting for electron correlation is more crucial than accounting for spin-orbit effects in determining Δ<sub><i>f</i></sub>. These results highlight the power of DMC for benchmarking 2D material physics and emphasize the importance of using beyond-DFT methods for studying 2D materials.</p>

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A many-body characterization of the fundamental gap in monolayer CrI3

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年1月16日

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  • Daniel Staros,
  • Abdulgani Annaberdiyev,
  • Kevin Gasperich,
  • Anouar Benali,
  • Panchapakesan Ganesh,
  • Brenda Rubenstein

摘要

Many-body fermionic Diffusion Monte Carlo (DMC) methods are applied to accurately predict the fundamental gap of the monolayer ferromagnet CrI3. The fundamental gap obtained, Δf = 2.9(1) eV, agrees well with the highest peak in optical spectroscopy measurements and a previous GW result. We numerically show that the same value of Δf is obtained in the thermodynamic limit using both neutral promotions and the standard definition of Δf based on the ionization potential and electron affinity. Analysis of the differences between density matrices of natural orbitals obtained from configuration interaction calculations explains why a single-reference trial wave function can produce an accurate excitation. We find that accounting for electron correlation is more crucial than accounting for spin-orbit effects in determining Δf. These results highlight the power of DMC for benchmarking 2D material physics and emphasize the importance of using beyond-DFT methods for studying 2D materials.