Bandgap of two-dimensional materials: Thorough assessment of modern exchange–correlation functionals

Tran, Fabien; Doumont, Jan; Kalantari, Leila; Blaha, Peter; Rauch, Tomáš; Borlido, Pedro; Botti, Silvana; Marques, Miguel A. L.; Patra, Abhilash; Jana, Subrata; Samal, Prasanjit

doi:10.1063/5.0059036

Cited by 34 publications

(32 citation statements)

References 86 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Finally, we also mention that the implementation has recently been used for the calculation of the band gap of 2D materials in Refs. [124,125].…”

Section: Discussionmentioning

confidence: 99%

Implementation of self-consistent MGGA functionals in augmented plane wave based methods

Doumont,

Tran,

Blaha

2021

Preprint

Self Cite

View full text Add to dashboard Cite

Functionals of the meta-generalized gradient approximation (MGGA) are nowadays widely used in chemistry and solid-state physics for the simulation of electronic systems like molecules, solids, or surfaces. Due to their dependency on the kinetic energy density, they are in principle more accurate than GGA functionals for various properties (geometry, binding energy, electronic structure, etc.), while being nearly as fast since they are still of the semilocal form. Thus, when an accuracy better than GGA is required, one may consider using a MGGA instead of the much more costly hybrid functionals or methods like the random-phase approximation or GW . In this work, the self-consistent implementation of MGGA functionals in APW based methods is presented. Technical aspects of the implementation are discussed, and calculations of band gaps, lattice constants, and magnetic moments are presented in order to validate our implementation. To test the changes of the electron density due to a MGGA, the electric field gradient on transition-metal atoms is calculated.

show abstract

“…Finally, we also mention that the implementation has recently been used for the calculation of the band gap of 2D materials in Refs. [124,125].…”

Section: Discussionmentioning

confidence: 99%

Implementation of self-consistent MGGA functionals in augmented plane wave based methods

Doumont,

Tran,

Blaha

2021

Preprint

Self Cite

View full text Add to dashboard Cite

show abstract

“…Recent efforts have focused on optimizing functionals to treat 2D systems (mostly layered compounds) and compared with theoretical benchmarks. [ 42,47,48 ]…”

Section: Introductionmentioning

confidence: 99%

“…DFT calculations are the most widely used and accepted ab initio theoretical method employed for solid materials. [38][39][40][41][42][43][44][45][46][47][48][49][50][51][52] This is an effective one-electron calculation that considers the total electron density and treats electron X-C, as a local, semilocal, or hybrid functional. This functional depends only on the electron density and is not dependent on the distinct nature of the electron states involved.…”

Section: Introductionmentioning

confidence: 99%

“…Recent efforts have focused on optimizing functionals to treat 2D systems (mostly layered compounds) and compared with theoretical benchmarks. [42,47,48] Limitations of DFT calculations are well recognized for systems with more localized electrons, such as semiconductors and oxides, [49][50][51][52] and except for a few cases, [53][54][55] have been largely overlooked in calculations of semiconductor surfaces and 2D silicenes. In the case of organic semiconducting materials [56,57] and π-bonded or conjugated systems [58][59][60][61][62] or systems with significant charge transfer, [56,57] these limitations are well established.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Evidence for “Unusual” Exchange–Correlation on Si(111) 7 × 7: Limitations of Density Functional Calculations for Charge Transfer Interactions on Semiconductor Surfaces

Demuth

2022

Physica Status Solidi (b)

View full text Add to dashboard Cite

Electron–electron interactions on the Si (111) surface associated with inaccuracies in treating exchange and correlation are shown to be consistent with discrepancies found between density functional calculations and experimental measurements of the 7 × 7 surface. Here, the measured filled and empty surface states of the 7 × 7 surface are shown to be shifted away from one another relative to those predicted by effective one electron calculations using density functional theory. This corresponds to the “energy gap problem” widely known to occur in most bulk semiconductors arising from the approximate treatment of electron exchange–correlation, X–C, within such theoretical constructs. Considering more realistic treatments of X–C to correct these energy shifts leads to a different interpretation of the surface states and a new interaction that stabilizes the 7 × 7. This provides a physical basis for its unusual properties some of which are also observed in related 2D systems. The effects of various electron–electron interactions from these new interactions are considered and their behavior is used to explain the metallic nature of the 7 × 7 at 300 K.

show abstract

“…Within those recent meta-GGAs, there are the functionals constructed from the cuspless hydrogen model [(r)MGGAC] 58,61 that show potential promising accuracy for different challenging problems in solid-state physics 50,60,61 . It is also quite an efficient semilocal functional that can predict band gaps of bulk and layered solids with reasonable accuracy 50,[61][62][63][64] .…”

Section: Introductionmentioning

confidence: 99%

Correct and accurate polymorphic energy ordering of transition-metal monoxides obtained from semilocal and onsite-hybrid exchange-correlation approximations

Ghosh¹,

Jana²,

Niranjan³

et al. 2021

Preprint

Self Cite

View full text Add to dashboard Cite

The relative energetic stability of the structural phases of common antiferromagnetic transitionmetal oxides (MnO, FeO, CoO, and NiO) within the semilocal and hybrid density functionals are fraught with difficulties. In particular, MnO is known to be the most difficult case for almost all common semilocal and hybrid density approximations. Here, we show that the meta-generalized gradient approximation (meta-GGA) constructed from the cuspless hydrogen model and Pauli kinetic energy density (MGGAC) can lead to the correct ground state of MnO. The relative energy differences of zinc-blende (zb) and rock-salt (rs) structures as computed using MGGAC are found to be in nice agreement with those obtained from high-level correlation methods like the random phase approximation or quantum Monte Carlo techniques. Besides, we have also applied the onsite hybrid functionals (closely related to DFT+U ) based on GGA and meta-GGA functionals, and it is shown that a relatively high amount of Hartree-Fock exchange is necessary to obtain the correct groundstate structure. Our present investigation suggests that the semilocal MGGAC and onsite hybrids, both being computationally cheap, as methods of choice for the calculation of the relative stability of antiferromagnetic transition-metal oxides having potential applications in solid-state physics and structural chemistry.

show abstract

Bandgap of two-dimensional materials: Thorough assessment of modern exchange–correlation functionals

Cited by 34 publications

References 86 publications

Implementation of self-consistent MGGA functionals in augmented plane wave based methods

Implementation of self-consistent MGGA functionals in augmented plane wave based methods

Evidence for “Unusual” Exchange–Correlation on Si(111) 7 × 7: Limitations of Density Functional Calculations for Charge Transfer Interactions on Semiconductor Surfaces

Correct and accurate polymorphic energy ordering of transition-metal monoxides obtained from semilocal and onsite-hybrid exchange-correlation approximations

Contact Info

Product

Resources

About