Accuracy of the Heyd-Scuseria-Ernzerhof hybrid functional to describe many-electron interactions and charge localization in semiconductors

Flores, Mauricio A.; Orellana, Walter; Menéndez-Proupín, E.

doi:10.1103/physrevb.98.155131

Cited by 16 publications

(7 citation statements)

References 119 publications

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“…Many examples which are expected to show analogous resonances have been reported in the literature. These include the negative carbon vacancy in 4H-SiC [16], or the cadmium vacancy in CdTe [23].…”

Section: Discussionmentioning

confidence: 99%

“…Despite being less refined, this approximation is similar to using DFT/pseudopotential pre-relaxed geometries for the calculation of Mössbauer parameters using all-electron full-potential methods [20]. This approach has also been used to obtain the formation energy and electronic structure of defects using Hedin's GW method [21,22] or diffusion quantum Monte Carlo [23]. Again, the above practice raises the question: can we actually rely on energies of state-of-the-art calculations that employ local-DFT geometries?…”

Section: Introductionmentioning

confidence: 99%

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Can we rely on hybrid-DFT energies of solid-state problems with local-DFT geometries?

Gouveia

Coutinho

2019

Electron. Struct.

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Hybrid functionals often improve considerably the accuracy of density-functional calculations, in particular of quantities resulting from the band structure. In plane-wave (PW) calculations this benefit comes at the cost of an increase in computation time by several orders of magnitude. For this reason, large-scale problems addressed within the PW formalism have to rely on pre-relaxed atomistic geometries, obtained with cheaper local or semi-local exchange-correlation functionals. We investigate how suitable these geometries are when plugged into single-point hybrid-DFT calculations. Based on several case studies, we find two important sources of error originating from (i) bond strain and (ii) over-mixing between defect and crystalline states. The first arises from the mismatch between the prerelaxed geometry and that obtained after a subsequent hybrid-DFT-level relaxation. The second occurs when defect states edging an underestimated band gap artificially mix with crystalline states, affecting the local bonding character of the defect, and therefore leading the spurious hybrid-DFT energies. Due to cancelation effects, the lingering strain contributes little ( 10 meV) to the error bar of quantities based on energy differences of pre-relaxed structures. The error from state over-mixing does not benefit from cancelation effects and has to be monitored with caution. Published in Electronic Structure 1, 015008 (2019).

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Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Can we rely on hybrid-DFT energies of solid-state problems with local-DFT geometries?

Gouveia

Coutinho

2019

Electron. Struct.

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“…Hybrid functionals, which mix a fraction of Hartree− Fock exchange with the local or semilocal exchange, have become increasingly popular in quantum chemistry and computational materials science because of the description of a more precise or accurate electronic band gap, which reaches closer to experimentally measured band gaps. Flores et al 58 assessed the accuracy of the HSE hybrid functional to describe many-electron interactions and charge localization in semiconductors. They have found the HSE functional to accurately describe many-electron interactions with moderate correlations.…”

Section: ■ Methodsmentioning

confidence: 99%

Ultrahigh Out-of-Plane Piezoelectricity Meets Giant Rashba Effect in 2D Janus Monolayers and Bilayers of Group IV Transition-Metal Trichalcogenides

Ahammed¹,

Jena²,

Rawat³

et al. 2020

J. Phys. Chem. C

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The simultaneous occurrence of gigantic piezoelectricity and Rashba effect in two-dimensional (2D) materials is unusually scarce. Inversion symmetry occurring in MX3 (M = Ti, Zr, Hf; X = S, Se) monolayers is broken upon constructing their Janus monolayer structures MX2Y (X ≠ Y =S, Se), thereby inducing a large out-of-plane piezoelectric constant d 33 (∼68 pm/V) in them. d 33 can be further enhanced to a super high value of ∼1000 pm/V upon applying vertical compressive strain in the van der Waals bilayers constituted by interfacing these Janus monolayers. Therefore, d 33 in these Janus transition-metal trichalcogenide (TMTC) bilayers reach more than 4-fold times that of bulk ceramic PZT material (∼268 pm/V). The absence of a horizontal mirror symmetry and the presence of strong spin–orbit coupling cause Rashba spin-splitting in electronic bands in these Janus 2D monolayers, which shows up as an ultrahigh Rashba parameter, αR ∼ 1.1 eV Å. It can be raised to 1.41 eV Å via compressive strain. Most of the 2D materials reported to date mainly show in-plane electric polarization, which severely limits their prospects in piezotronic devices. In this present work, the piezoelectricity shown by the Janus monolayers of group IV TMTCs and their bilayers is significantly higher than the ones generally utilized in the form of three-dimensional bulk piezoelectric solids, for example, α-quartz (d 11 = 2.3 pm/V), wurtzite-GaN (d 33 = 3.1 pm/V), and wurtzite-AlN (d 33 = 5.6 pm/V). It is exceedingly higher than that in Janus multilayer/bulk structures of Mo- and W-based transition-metal dichalcogenides, for example, MoSTe (d 33 ∼ 10 pm/V). The 2D Janus TMTC monolayers and their bilayers reported herewith straddle giant Rashba spin-splitting and ultrahigh piezoelectricity, thereby making them immensely promising candidates in the next-generation electronics, piezotronics, spintronics, flexible electronics, and piezoelectric devices.

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“…Since periodic boundary conditions are applied in VASP, 20 Å interlayer spacing distance was set to prevent the interaction among the periodic images. To study electronic band structure, in addition to GGA-PBE functional, Heyd-Scuseria-Ernzerhof hybrid functional (HSE06) [70] has been employed to calculate a more precise band-gap [71]. The Phonopy code [72] conjugated with VASP was employed to compute phonon dispersion modes.…”

Section: Computational Detailsmentioning

confidence: 99%

Piezoelectricity in two-dimensional aluminum, boron and Janus aluminum-boron monochalcogenide monolayers

Choopani¹,

Alyörük²

2022

J. Phys. D: Appl. Phys.

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Piezoelectricity is a property of a material that converts mechanical energy into electrical energy or vice versa. It is known that group-III monochalcogenides, including GaS, GaSe, and InSe, show piezoelectricity in their monolayer form. Piezoelectric coefficients of these monolayers are the same order of magnitude as the previously discovered two-dimensional (2D) piezoelectric materials such as boron nitride (BN) and molybdenum disulfide (MoS2) monolayers. Considering a series of monolayer monochalcogenide structures including boron and aluminum (MX, M =B, Al, X = O, S, Se, Te), we design a series of derivative Janus structures (AlBX2, X = O, S, Se, Te). Ab-initio density functional theory (DFT) and density functional perturbation theory (DFPT) calculations are carried out systematically to predict their structural, electronic, electromechanical and phonon dispersion properties. The electronic band structure analysis indicate that all these 2D materials are semiconductors. The absence of imaginary phonon frequencies in phonon dispersion curves demonstrate that the systems are dynamically stable. In addition, this study shows that these materials exhibit outstanding piezoelectric properties. For AlBO2 monolayer with the relaxed-ion piezoelectric coefficients, d11=15.89(15.87) pm/V and d31=0.52(0.44) pm/V, the strongest piezoelectric properties were obtained. It has large in-plane and out-of-plane piezoelectric coefficients that are comparable to or larger than those of previously reported non-Janus monolayer structures such as MoS2 and GaSe, and also Janus monolayer structures including: In2SSe, Te2Se, MoSeTe, InSeO, SbTeI, and ZrSTe. These results, together with the fact that a lot of similar 2D systems have been synthesized so far, demonstrate the great potential of these materials in nanoscale electromechanical applications.

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Accuracy of the Heyd-Scuseria-Ernzerhof hybrid functional to describe many-electron interactions and charge localization in semiconductors

Cited by 16 publications

References 119 publications

Can we rely on hybrid-DFT energies of solid-state problems with local-DFT geometries?

Can we rely on hybrid-DFT energies of solid-state problems with local-DFT geometries?

Ultrahigh Out-of-Plane Piezoelectricity Meets Giant Rashba Effect in 2D Janus Monolayers and Bilayers of Group IV Transition-Metal Trichalcogenides

Piezoelectricity in two-dimensional aluminum, boron and Janus aluminum-boron monochalcogenide monolayers

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