Transferable screened range-separated hybrids for layered materials: The cases of<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:msub><mml:mi>MoS</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:math>and h-BN

Ramasubramaniam, Ashwin; Wing, Dahvyd; Kronik, Leeor

doi:10.1103/physrevmaterials.3.084007

Cited by 27 publications

(23 citation statements)

References 78 publications

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“…Similarly, optimally-tuned range-separated functionals have been shown to provide band structures in quantitative agreement with GW results for freestanding MoS 2 19 , in agreement with our results, as shown in Fig. S3 (our optimized values are α, γ = (0.1, 0.0245Bohr −1 ) as compared with α, γ = (0.106, 0.02Bohr −1 ) of Ref.…”

Section: B Electronic Structure Of Freestanding Mos2supporting

confidence: 90%

“…Range-separated hybrid functionals allow for accurate self-consistent calculations through the generation of a system-dependent set of physical parameters. Previous works have shown that a physicallyconstraint, parameter-free tuning of these functionals can lead to quantitatively accurate predictions of the electronic and optical properties of various materials, including organic 17 and inorganic 18 solids, as well as 2D materials 19 . However, the applicability of these functionals and optimization criteria to multi-component and mixed-dimensional systems such as MDHJs remains an open question.…”

Section: Introductionmentioning

confidence: 99%

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Range-Separated Hybrid Functionals for Mixed-Dimensional Heterojunctions: Application to Phthalocyanines/MoS2

Zhou¹,

Liu²,

Marks³

et al. 2021

Preprint

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We analyze the electronic structure and level alignment of transition-metal phthalocyanine (MPc) molecules adsorbed on two-dimensional MoS 2 employing density functional theory (DFT) calculations. We develop a procedure for multi-objective optimal tuning of parameters of range-separated hybrid functionals in these mixed-dimensional systems. Using this procedure, which leads to the asymptotically-correct exchangecorrelation potential between molecule and two-dimensional material, we obtain electronic structures consistent with experimental photoemission results for both energy level alignment and electronic bandgaps, representing a significant advance compared to standard DFT methods. We elucidate the MoS 2 valence resonance with the transition-metal phthalocyanine non-frontier 3d orbitals and its dependence on the transition metal atomic number. Based on our calculations, we derive parameter-free, model self-energy corrections to semi-local DFT that quantitatively accounts for the effects of the heterogeneous dielectric environment on the electronic structure of these mixed-dimensional heterojunctions, highlighting the importance of non-local corrections for d-states of MPcs, which are correctly described by OT-RSH functionals in addition to the dielectric screening model. IL 60208, USA d)

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Section: B Electronic Structure Of Freestanding Mos2supporting

confidence: 90%

Section: Introductionmentioning

confidence: 99%

Range-Separated Hybrid Functionals for Mixed-Dimensional Heterojunctions: Application to Phthalocyanines/MoS2

Zhou¹,

Liu²,

Marks³

et al. 2021

Preprint

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“…In particular, the so-called optimally tuned range-separated hybrids produce excellent results for organic molecular crystals [54,55]. Recently, Wing and co-workers [56,57] showed that range-separated hybrids with an empirical parameter agree well with GW BSE results for several materials.…”

Section: Introductionmentioning

confidence: 94%

“…While hybrid functionals have found widespread application for periodic solids due mainly to their excellent performance for calculating band gaps [37][38][39][40][41][42][43][44][45][46][47][48][49], there have so far been relatively few applications of hybrid functionals for optical spectra in semiconductors and insulators [50][51][52][53][54][55][56][57].…”

Section: B From the Simplified Bse To Generalized Tddft: A Hybrid Fumentioning

confidence: 99%

Low-cost alternatives to the Bethe-Salpeter equation: Towards simple hybrid functionals for excitonic effects in solids

Sun

Yang

Ullrich

2020

Phys. Rev. Research

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The Bethe-Salpeter equation (BSE) is the standard computational method for optical excitations in solids, including excitonic effects. In this paper we explore ways to reduce the computational cost of the BSE by simplifying the dielectrically screened Coulomb interaction: Instead of calculating the dielectric function from first principles, we replace it by a momentum-dependent model dielectric function or just by a single parameter. Combined with a semilocal exchange-correlation kernel, this defines an alternative class of hybrid functionals for solids within generalized time-dependent density-functional theory. We perform a systematic assessment of these simplified approaches and find that they yield optical absorption spectra and exciton binding energies of semiconductors and wide-gap insulators in close agreement with the standard BSE and with experiment. We also present applications to the perovskite material CsPbBr 3 as an example of a more complex system.

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“…It should be noted that the OT‐SRSH approach in the current form cannot be used for general solids with ionic or covalent bonding characters since the optimal tuning condition Equation ) cannot be applied easily for extended systems. It is, however, interesting to mention recent works by Kronik and workers, 109,150,151 in which the SRSH functional with the range separation parameter μ determined by either fitting experimental band gaps, 109 or GW band gaps at one specific high‐symmetry point of the Brillouin zone, 150 when applied in the TDDFT framework, was found to be able to predict optical spectra of several prototypical covalent and ionic solids in good agreement with GW + BSE.…”

Section: Recent Methodological Developmentsmentioning

confidence: 93%

Hybrid functionals with system‐dependent parameters: Conceptual foundations and methodological developments

Zhang

Cui

Wang

et al. 2020

WIREs Comput Mol Sci

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Approximate density-functional theory (DFT) has become the major workhorse of modern computational chemistry and materials science, but the most widely used DFT approaches, local-density approximation (LDA) and generalized gradient approximation (GGA), suffer from some fundamental deficiencies, including, in particular, the band gap problem. As a relatively cheap way to overcome the difficulty confronted by LDA/GGA, hybrid functional methods have attracted tremendous interest, first in molecular quantum chemistry, and more recently also in computational materials science. While early hybrid functionals use fixed parameters that are determined either by fitting some standard experimental database or based on theoretical arguments, recent studies have clearly indicated that the hybridization parameters carry on the physical significance and therefore should be system-dependent. Developing theoretical methods to evaluate those parameters in a first-principles manner has become one of the most active frontiers in theoretical chemistry community, and various schemes have been proposed. In this article, we aim at giving a systematic overview on the main theoretical concepts underlying various strategies and review major methodological developments in the recent years.

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Transferable screened range-separated hybrids for layered materials: The cases ofMoS2and h-BN

Cited by 27 publications

References 78 publications

Range-Separated Hybrid Functionals for Mixed-Dimensional Heterojunctions: Application to Phthalocyanines/MoS2

Range-Separated Hybrid Functionals for Mixed-Dimensional Heterojunctions: Application to Phthalocyanines/MoS2

Low-cost alternatives to the Bethe-Salpeter equation: Towards simple hybrid functionals for excitonic effects in solids

Hybrid functionals with system‐dependent parameters: Conceptual foundations and methodological developments

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