Relative stability of FeS<sub>2</sub>polymorphs with the random phase approximation approach

Zhang, Min-Ye; Cui, Zhi-Hao; Jiang, Hong

doi:10.1039/c8ta00759d

Cited by 26 publications

(31 citation statements)

References 92 publications

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“…The latter study established that functions of the surface ligands affect the stability of FeS 2 (FeS 2 nanorods synthesized in laboratory) (Barand and Russo, 2009 ). The stability of FeS contributed to low energy excitation from Fe d to S-Sσ * p (Zhang et al, 2018 ). Fe 3 S 4 was observed at 200°C for 30 h then it transformed to FeS 2 over time (Gao et al, 2015 ).…”

Section: Characteristics Of Nano-sized Iron Sulfidesmentioning

confidence: 99%

“…In addition, the phases of iron sulfide in nature include mackinawite (FeS), pyrrhotite (Fe 1−x S), pyrite (FeS 2 ), and greigite (Fe 3 S 4 ), etc., which exhibit more variability than iron oxide containing only Fe 2 O 3 and Fe 3 O 4 . The band gap in iron sulfide is smaller than that of iron oxide, leading to the former having more appropriate electron transfer and conductivity (Wadia et al, 2009 ; Jin et al, 2017 ; Zhang et al, 2018 ). Importantly, iron-sulfur clusters are important cofactors in many enzymes which serve as active centers for electron transfer in catalytic processes and respiratory chain reactions (Qi and Cowan, 2011 ).…”

Section: Introductionmentioning

confidence: 99%

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Nano-Sized Iron Sulfide: Structure, Synthesis, Properties, and Biomedical Applications

2020

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Nano-sized iron sulfides have attracted intense research interest due to the variety of their types, structures, and physicochemical properties. In particular, nano-sized iron sulfides exhibit enzyme-like activity by mimicking natural enzymes that depend on an iron-sulfur cluster as cofactor, extending their potential for applications in biomedicine. The present review principally summarizes the synthesis, properties and applications in biomedical fields, demonstrating that nano-sized iron sulfides have considerable potential for improving human health and quality of life.

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Section: Characteristics Of Nano-sized Iron Sulfidesmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Nano-Sized Iron Sulfide: Structure, Synthesis, Properties, and Biomedical Applications

2020

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“…An entirely discrete challenge for functionals is the ground state structure prediction problem because a ground state is either correctly stabilized or not. Only a limited number of case studies are available in the recent literature where SCAN is benchmarked on structure selection, focusing on MnO2 [20], FeS2 [21], Ce2O3, Mn2O3, Fe3O4 [22], TiO2 [23], as well as broad benchmarking work [24] on binary main group compounds observing that SCAN is more accurate than PBE in ground state structure prediction. However, there is no established rationalization of the origin of structure prediction accuracy given by the SCAN functional, except in systems where self-interaction is a known problem which can be addressed otherwise through a Hubbard U correction or higher order methods.…”

Section: Introductionmentioning

confidence: 99%

Rationalizing accurate structure prediction in the meta-GGA SCAN functional

2019

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The ability of first-principles computational methods to reproduce ground-state crystal structure selection is key to their application in the discovery of new materials, and yet presents a formidable challenge due to the low energy scale of the problem and lack of systematic error cancellation. The recently-developed Strongly Constrained and Appropriately Normed (SCAN) functional is notable for accurately calculating physical properties such as formation energies and in particular, correctly predicting ground state structures. Here, we attempt to rationalize the improved structure prediction accuracy in SCAN by investigating the relationship between preferred coordination environments, the description of attractive van der Waals (vdW) interactions, and the overall ground state prediction in bulk main group solids. We observe a systematic under-coordination error in the traditional Perdew, Burke, and Ernzerhof (PBE) functional which is not present in SCAN results and find that semi-empirical dispersion corrections in the form of PBE+D3 fail to correct this error in a consistent or physical manner. We conclude that the medium-range vdW interaction is correctly parameterized in SCAN and yields meaningful relative energies between coordination environments.

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“…However, the error can be detrimental to the numerical accuracy of methods where the summation over unoccupied states is required, e.g. GW and DFT methods with density approximations belonging to the fifth rung of Jacobi ladder ( Perdew and Schmidt, 2001 ) such as the adiabatic-connection dissipation-fluctuation (ACFD) calculation under RPA for ground-state energy ( Ren et al, 2012 ; Cui et al, 2016 ; Zhang et al, 2018 ). In these methods, the completeness of summation and quality of unoccupied states play a crucial role.…”

Section: Theory and Methodsmentioning

confidence: 99%

Accurate Prediction of Band Structure of FeS2: A Hard Quest of Advanced First-Principles Approaches

Zhang

Jiang

2021

Front. Chem.

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The pyrite and marcasite polymorphs of FeS2 have attracted considerable interests for their potential applications in optoelectronic devices because of their appropriate electronic and optical properties. Controversies regarding their fundamental band gaps remain in both experimental and theoretical materials research of FeS2. In this work, we present a systematic theoretical investigation into the electronic band structures of the two polymorphs by using many-body perturbation theory with the GW approximation implemented in the full-potential linearized augmented plane waves (FP-LAPW) framework. By comparing the quasi-particle (QP) band structures computed with the conventional LAPW basis and the one extended by high-energy local orbitals (HLOs), denoted as LAPW + HLOs, we find that one-shot or partially self-consistent GW (G0W0 and GW0, respectively) on top of the Perdew-Burke-Ernzerhof (PBE) generalized gradient approximation with a converged LAPW + HLOs basis is able to remedy the artifact reported in the previous GW calculations, and leads to overall good agreement with experiment for the fundamental band gaps of the two polymorphs. Density of states calculated from G0W0@PBE with the converged LAPW + HLOs basis agrees well with the energy distribution curves from photo-electron spectroscopy for pyrite. We have also investigated the performances of several hybrid functionals, which were previously shown to be able to predict band gaps of many insulating systems with accuracy close or comparable to GW. It is shown that the hybrid functionals considered in general fail badly to describe the band structures of FeS2 polymorphs. This work indicates that accurate prediction of electronic band structure of FeS2 poses a stringent test on state-of-the-art first-principles approaches, and the G0W0 method based on semi-local approximation performs well for this difficult system if it is practiced with well-converged numerical accuracy.

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Relative stability of FeS₂polymorphs with the random phase approximation approach

Abstract: We highlight the role of electron correlation in the correct prediction of the relative stability of FeS2polymorphs by ACFDT-RPA.

Cited by 26 publications

References 92 publications

Nano-Sized Iron Sulfide: Structure, Synthesis, Properties, and Biomedical Applications

Nano-Sized Iron Sulfide: Structure, Synthesis, Properties, and Biomedical Applications

Rationalizing accurate structure prediction in the meta-GGA SCAN functional

Accurate Prediction of Band Structure of FeS2: A Hard Quest of Advanced First-Principles Approaches

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Relative stability of FeS2polymorphs with the random phase approximation approach

Abstract: We highlight the role of electron correlation in the correct prediction of the relative stability of FeS2polymorphs by ACFDT-RPA.

Cited by 26 publications

References 92 publications

Nano-Sized Iron Sulfide: Structure, Synthesis, Properties, and Biomedical Applications

Nano-Sized Iron Sulfide: Structure, Synthesis, Properties, and Biomedical Applications

Rationalizing accurate structure prediction in the meta-GGA SCAN functional

Accurate Prediction of Band Structure of FeS2: A Hard Quest of Advanced First-Principles Approaches

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Product

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About

Relative stability of FeS₂polymorphs with the random phase approximation approach