<p>We employ cluster extension of dynamical mean-field theory (CDMFT) to systematically investigate the impact of double counting corrections on the correlated electronic structure of La<sub>3</sub>Ni<sub>2</sub>O<sub>7</sub> under ambient pressure. By adjusting double-counting parameters, while maintaining a fixed Fermi surface, we observe a pronounced orbital-selective density of states change: the <InlineEquation ID="IEq1"> <EquationSource Format="TEX">\(d_{z^2}\)</EquationSource> <EquationSource Format="MATHML"><math> <msub> <mi>d</mi> <msup> <mi>z</mi> <mn>2</mn> </msup> </msub> </math></EquationSource> </InlineEquation> orbital undergoes significant variation near the Fermi level with increasing <InlineEquation ID="IEq2"> <EquationSource Format="TEX">\(E_{dc}^z\)</EquationSource> <EquationSource Format="MATHML"><math> <msubsup> <mi>E</mi> <mrow> <mi mathvariant="italic">dc</mi> </mrow> <mi>z</mi> </msubsup> </math></EquationSource> </InlineEquation>, while the <InlineEquation ID="IEq3"> <EquationSource Format="TEX">\(d_{x^2-y^2}\)</EquationSource> <EquationSource Format="MATHML"><math> <msub> <mi>d</mi> <mrow> <msup> <mi>x</mi> <mn>2</mn> </msup> <mo>-</mo> <msup> <mi>y</mi> <mn>2</mn> </msup> </mrow> </msub> </math></EquationSource> </InlineEquation> orbital remains essentially unchanged throughout the entire range. Analysis of renormalization factor show the monotonic dependence with double counting in both <InlineEquation ID="IEq4"> <EquationSource Format="TEX">\(d_{z^2}\)</EquationSource> <EquationSource Format="MATHML"><math> <msub> <mi>d</mi> <msup> <mi>z</mi> <mn>2</mn> </msup> </msub> </math></EquationSource> </InlineEquation> and <InlineEquation ID="IEq5"> <EquationSource Format="TEX">\(d_{x^2-y^2}\)</EquationSource> <EquationSource Format="MATHML"><math> <msub> <mi>d</mi> <mrow> <msup> <mi>x</mi> <mn>2</mn> </msup> <mo>-</mo> <msup> <mi>y</mi> <mn>2</mn> </msup> </mrow> </msub> </math></EquationSource> </InlineEquation> orbital, and it also identifies an optimal double counting window in <InlineEquation ID="IEq6"> <EquationSource Format="TEX">\(d_{z^2}\)</EquationSource> <EquationSource Format="MATHML"><math> <msub> <mi>d</mi> <msup> <mi>z</mi> <mn>2</mn> </msup> </msub> </math></EquationSource> </InlineEquation> orbital aligns with experimental values. We also find the interlayer Matsubara self energy exhibits non-monotonic dependence on <InlineEquation ID="IEq7"> <EquationSource Format="TEX">\(E_{dc}^z\)</EquationSource> <EquationSource Format="MATHML"><math> <msubsup> <mi>E</mi> <mrow> <mi mathvariant="italic">dc</mi> </mrow> <mi>z</mi> </msubsup> </math></EquationSource> </InlineEquation>, deviating from theoretical predictions. This anomaly is attributed to the metallization of oxygen-bridged pathways, which disrupts the prerequisite for charge transfer via apical oxygen. Our results establish <InlineEquation ID="IEq8"> <EquationSource Format="TEX">\(E_{dc}\)</EquationSource> <EquationSource Format="MATHML"><math> <msub> <mi>E</mi> <mrow> <mi mathvariant="italic">dc</mi> </mrow> </msub> </math></EquationSource> </InlineEquation> as a critical control parameter for correlated electronic structure in La<sub>3</sub>Ni<sub>2</sub>O<sub>7</sub> and provide a computational framework for resolving orbital-dependent correlation effects in layered materials.</p>

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Evolution of correlated electrons in La3Ni2O7 at ambient pressure: a study of double-counting effect

  • Zhongyi Xie,
  • Zhihui Luo,
  • Wei Wu,
  • Daoxin Yao

摘要

We employ cluster extension of dynamical mean-field theory (CDMFT) to systematically investigate the impact of double counting corrections on the correlated electronic structure of La3Ni2O7 under ambient pressure. By adjusting double-counting parameters, while maintaining a fixed Fermi surface, we observe a pronounced orbital-selective density of states change: the \(d_{z^2}\) d z 2 orbital undergoes significant variation near the Fermi level with increasing \(E_{dc}^z\) E dc z , while the \(d_{x^2-y^2}\) d x 2 - y 2 orbital remains essentially unchanged throughout the entire range. Analysis of renormalization factor show the monotonic dependence with double counting in both \(d_{z^2}\) d z 2 and \(d_{x^2-y^2}\) d x 2 - y 2 orbital, and it also identifies an optimal double counting window in \(d_{z^2}\) d z 2 orbital aligns with experimental values. We also find the interlayer Matsubara self energy exhibits non-monotonic dependence on \(E_{dc}^z\) E dc z , deviating from theoretical predictions. This anomaly is attributed to the metallization of oxygen-bridged pathways, which disrupts the prerequisite for charge transfer via apical oxygen. Our results establish \(E_{dc}\) E dc as a critical control parameter for correlated electronic structure in La3Ni2O7 and provide a computational framework for resolving orbital-dependent correlation effects in layered materials.