DFT+U and quantum Monte Carlo study of electronic and optical properties of AgNiO2 and AgNi1−xCoxO2 delafossite

Hyeondeok Shin; Panchapakesan Ganesh; Paul R.C. Kent; Anouar Benali; Anand Bhattacharya; Ho Nyung Lee; Olle Heinonen; Jaron T. Krogel

doi:10.1039/d3cp03477a

DFT+U and quantum Monte Carlo study of electronic and optical properties of AgNiO₂ and AgNi_1−xCo_xO₂ delafossite

Hyeondeok Shin, Panchapakesan Ganesh, Paul R.C. Kent, Anouar Benali, Anand Bhattacharya, Ho Nyung Lee, Olle Heinonen, Jaron T. Krogel

Research output: Contribution to journal › Article › peer-review

Abstract

As the only semimetallic d¹⁰-based delafossite, AgNiO₂ has received a great deal of attention due to both its unique semimetallicity and its antiferromagnetism in the NiO₂ layer that is coupled with a lattice distortion. In contrast, other delafossites such as AgCoO₂ are insulating. Here we study how the electronic structure of AgNi_1−xCo_xO₂ alloys vary with Ni/Co concentration, in order to investigate the electronic properties and phase stability of the intermetallics. While the electronic and magnetic structure of delafossites have been studied using density functional theory (DFT), earlier studies have not included corrections for strong on-site Coulomb interactions. In order to treat these interactions accurately, in this study we use Quantum Monte Carlo (QMC) simulations to obtain accurate estimates for the electronic and magnetic properties of AgNiO₂. By comparison to DFT results we show that these electron correlations are critical to account for. We show that Co doping on the magnetic Ni sites results in a metal-insulator transition near x ∼0.33, and reentrant behavior near x ∼ 0.66.

Original language	English
Pages (from-to)	6967-6976
Number of pages	10
Journal	Physical Chemistry Chemical Physics
Volume	26
Issue number	8
DOIs	https://doi.org/10.1039/d3cp03477a
State	Published - Feb 6 2024

Funding

This work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, as part of the Computational Materials Sciences Program and Center for Predictive Simulation of Functional Materials. An award of computer time was provided by the Innovative and Novel Computational Impact on Theory and Experiment (INCITE) program. This research used resources of the Argonne Leadership Computing Facility, which is a DOE Office of Science User Facility supported under contract DE-AC02-06CH11357 and resources of the Oak Ridge Leadership Computing Facility, which is a DOE Office of Science User Facility supported under Contract DE-AC05-00OR22725.

Funders	Funder number
U.S. Department of Energy
Office of Science	DE-AC05-00OR22725, DE-AC02-06CH11357
Basic Energy Sciences
Division of Materials Sciences and Engineering

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10.1039/d3cp03477a

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title = "DFT+U and quantum Monte Carlo study of electronic and optical properties of AgNiO2 and AgNi1−xCoxO2 delafossite",

abstract = "As the only semimetallic d10-based delafossite, AgNiO2 has received a great deal of attention due to both its unique semimetallicity and its antiferromagnetism in the NiO2 layer that is coupled with a lattice distortion. In contrast, other delafossites such as AgCoO2 are insulating. Here we study how the electronic structure of AgNi1−xCoxO2 alloys vary with Ni/Co concentration, in order to investigate the electronic properties and phase stability of the intermetallics. While the electronic and magnetic structure of delafossites have been studied using density functional theory (DFT), earlier studies have not included corrections for strong on-site Coulomb interactions. In order to treat these interactions accurately, in this study we use Quantum Monte Carlo (QMC) simulations to obtain accurate estimates for the electronic and magnetic properties of AgNiO2. By comparison to DFT results we show that these electron correlations are critical to account for. We show that Co doping on the magnetic Ni sites results in a metal-insulator transition near x ∼0.33, and reentrant behavior near x ∼ 0.66.",

author = "Hyeondeok Shin and Panchapakesan Ganesh and Kent, {Paul R.C.} and Anouar Benali and Anand Bhattacharya and Lee, {Ho Nyung} and Olle Heinonen and Krogel, {Jaron T.}",

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doi = "10.1039/d3cp03477a",

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T1 - DFT+U and quantum Monte Carlo study of electronic and optical properties of AgNiO2 and AgNi1−xCoxO2 delafossite

AU - Shin, Hyeondeok

AU - Ganesh, Panchapakesan

AU - Kent, Paul R.C.

AU - Benali, Anouar

AU - Bhattacharya, Anand

AU - Lee, Ho Nyung

AU - Heinonen, Olle

AU - Krogel, Jaron T.

PY - 2024/2/6

Y1 - 2024/2/6

N2 - As the only semimetallic d10-based delafossite, AgNiO2 has received a great deal of attention due to both its unique semimetallicity and its antiferromagnetism in the NiO2 layer that is coupled with a lattice distortion. In contrast, other delafossites such as AgCoO2 are insulating. Here we study how the electronic structure of AgNi1−xCoxO2 alloys vary with Ni/Co concentration, in order to investigate the electronic properties and phase stability of the intermetallics. While the electronic and magnetic structure of delafossites have been studied using density functional theory (DFT), earlier studies have not included corrections for strong on-site Coulomb interactions. In order to treat these interactions accurately, in this study we use Quantum Monte Carlo (QMC) simulations to obtain accurate estimates for the electronic and magnetic properties of AgNiO2. By comparison to DFT results we show that these electron correlations are critical to account for. We show that Co doping on the magnetic Ni sites results in a metal-insulator transition near x ∼0.33, and reentrant behavior near x ∼ 0.66.

AB - As the only semimetallic d10-based delafossite, AgNiO2 has received a great deal of attention due to both its unique semimetallicity and its antiferromagnetism in the NiO2 layer that is coupled with a lattice distortion. In contrast, other delafossites such as AgCoO2 are insulating. Here we study how the electronic structure of AgNi1−xCoxO2 alloys vary with Ni/Co concentration, in order to investigate the electronic properties and phase stability of the intermetallics. While the electronic and magnetic structure of delafossites have been studied using density functional theory (DFT), earlier studies have not included corrections for strong on-site Coulomb interactions. In order to treat these interactions accurately, in this study we use Quantum Monte Carlo (QMC) simulations to obtain accurate estimates for the electronic and magnetic properties of AgNiO2. By comparison to DFT results we show that these electron correlations are critical to account for. We show that Co doping on the magnetic Ni sites results in a metal-insulator transition near x ∼0.33, and reentrant behavior near x ∼ 0.66.

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DFT+U and quantum Monte Carlo study of electronic and optical properties of AgNiO₂ and AgNi_1−xCo_xO₂ delafossite

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