Screened-exchange density functional theory description of the electronic structure and phase stability of the chalcopyrite materials<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:msub><mml:mtext>AgInSe</mml:mtext><mml:mn>2</mml:mn></mml:msub></mml:math>and<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:msub><mml:mtext>AuInSe</mml:mtext><mml:mn>2</mml:mn></mml:msub></mml:math>

Kim, Namhoon; Martin, Pamela; Rockett, Angus; Ertekin, Elif

doi:10.1103/physrevb.93.165202

Cited by 12 publications

(23 citation statements)

References 41 publications

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“…Generally, they agree qualitatively, but in some cases the CuInSe 2 stability regions may differ remarkably from the other results, even among those calculated using the HSE06 functional. Our phase stability diagram is close to that calculated by Yee et al and also to those presented by Pohl and Albe, Huang et al, or Kim et al Due to a differing CuInSe 2 heat of formation, the chemical potential diagram by Bekaert et al has a noticeably bigger stability region than that in the present work.…”

Section: Point Defectsmentioning

confidence: 99%

First‐Principles Modeling of Point Defects and Complexes in Thin‐Film Solar‐Cell Absorber CuInSe₂

Malitckaya

Komsa

Havu

et al. 2017

Adv Elect Materials

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as the composition of the sample changes from Cu-rich to Cu-poor, so that in the Cupoor samples only one peak is detected. Although only the Cu-poor material is important for actual devices Cu-rich samples give indispensable information for defect identification.First-principles calculations based on the density functional theory (DFT) can be used to obtain important, complementary information about point defects such as formation energies and charge transition levels. [6] A plethora of studies concerning defects in CuInSe 2 and CuGaSe 2 has been published over the last two decades. [7][8][9][10][11][12][13] The most recent DFT investigations have employed hybrid functionals, which can overcome the energy band gap problem plaguing the older studies and can thus also provide information about the defect level positions within the band gap. [9][10][11][12][13] The results of different calculations agree well with respect to general trends in formation energies of the most important defects, such as the copper vacancy (V Cu ), indium antisite on copper place (In Cu ), and copper interstitial (Cu int ). However, the results differ in some important cases. For instance, there are clearly different values for the ionization levels within the band gap for the copper antisite on the indium place (Cu In ) and indium vacancy (V In ). Based on the formation energy calculations, V Cu and Cu In are abundant acceptors, and are most probably responsible for some of the above-mentioned PL peaks, but it is unclear whether any native defect can be responsible for the third acceptor level.One important goal of the present work was to gain a perspective on the present unsatisfactory situation in modeling point defects in CIGSe and to approach the ultimate accuracy by which DFT is able to predict the properties of bulk crystalline materials. [14] First we carried out a detailed benchmarking of the first-principles computational scheme used. We checked effects due to the supercell size and shape, as well as those of the finite-size supercell correction scheme. We used also two very different implementations of the first-principles DFT method, which differ in describing valence-core electron interaction and electron wave functions (see below). After finding the computational parameters yielding accurate results, we calculated formation energies and charge transition levels for different acceptor candidates in CuInSe 2 . By carefully considering the relevant chemical potential limits, we were able to draw conclusions about the abundances of different defects. In addition to simple native defects, we have also considered a set of complexes formed by them. Our paper is organized as follows.

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Section: Point Defectsmentioning

confidence: 99%

First‐Principles Modeling of Point Defects and Complexes in Thin‐Film Solar‐Cell Absorber CuInSe₂

Malitckaya

Komsa

Havu

et al. 2017

Adv Elect Materials

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“…Further, a significant shortcoming in standard DFT based methods is the presence of inherent self-interaction error (SIE) 14,70 . In the case of chalcopyrites, this shortcoming results in shallow d states description for the cations, and in general, the absence of derivative discontinuity in the KS bandgap which is defined as the difference between eigenvalues of the CBM and VBM.…”

Section: Electronic Propertiesmentioning

confidence: 99%

“…The absence of the LDA/GGA computed bandgaps in some of the chalcopyrites and other material systems has been attributed to large ratio of SIE in exchange functionals. Hybrid functionals eliminate some amount of SIE and improve the performance and estimates of bandgaps 14,70 . The performance of the meta-GGA functionals which are implemented in gKS scheme (such as SCAN and MGGAC), in providing estimates of the electronic properties of chalcopyrites has not been reported.…”

Section: Electronic Propertiesmentioning

confidence: 99%

“…In the case of HSE06, the relative bandgap enhancement compared to that for semilocal functionals happens because of the inclusion of the non-local HF exchange, which reduces the repulsion between Cu−3d and S−4p states and thereby results in the bandgap opening 70 . Importantly, the bandgap enlargement in the case of HSE06 as compared to other semilocal functionals (MGGAC, SCAN, TM, and PBE) may be attributed to (i) enlargement of bandwidth and the orbital spacing which directly influences the bandgap and (ii) the shift of non-bonding 3d states downward which reduce the p − d repulsion.…”

Section: Density Of Statesmentioning

confidence: 99%

“…The PBE and HSE06 results in Table II are taken from ref. 70 . As can be seen, the PBE underestimates the formation energies of both the chalcopyrites by more than 30%.…”

Section: Formation Enthalpiesmentioning

confidence: 99%

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Improved electronic structure prediction of chalcopyrite semiconductors from a semilocal density functional based on Pauli kinetic energy enhancement factor

Ghosh,

Jana,

Niranjan

et al. 2021

Preprint

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The correct treatment of d electrons is of prime importance in order to predict the electronic properties of the prototype chalcopyrite semiconductors. The effect of d states is linked with the anion displacement parameter u, which in turn influences the bandgap of these systems. Semilocal exchange-correlation functionals which yield good structural properties of semiconductors and insulators often fail to predict reasonable u because of the underestimation of the bandgaps arising from the strong interplay between d electrons. In the present study, we show that the meta-generalized gradient approximation (meta-GGA) obtained from the cuspless hydrogen density (MGGAC) [Phys. Rev. B 100, 155140 (2019)] performs in an improved manner in apprehending the key features of the electronic properties of chalcopyrites, and its bandgaps are comparative to that obtained using state-of-art hybrid methods. Moreover, the present assessment also shows the importance of the Pauli kinetic energy enhancement factor, α = (τ − τ W )/τ unif in describing the d electrons in chalcopyrites. The present study strongly suggests that the MGGAC functional within semilocal approximations can be a better and preferred choice to study the chalcopyrites and other solid-state systems due to its superior performance and significantly low computational cost.

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Investigation of Ag(Ga,In)Se2 as thin-film solar cell absorbers: A first-principles study

Wang¹,

Dou

Zheng

et al. 2022

Sci. China Phys. Mech. Astron.

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Screened-exchange density functional theory description of the electronic structure and phase stability of the chalcopyrite materialsAgInSe2andAuInSe2

Cited by 12 publications

References 41 publications

First‐Principles Modeling of Point Defects and Complexes in Thin‐Film Solar‐Cell Absorber CuInSe₂

First‐Principles Modeling of Point Defects and Complexes in Thin‐Film Solar‐Cell Absorber CuInSe₂

Improved electronic structure prediction of chalcopyrite semiconductors from a semilocal density functional based on Pauli kinetic energy enhancement factor

Investigation of Ag(Ga,In)Se2 as thin-film solar cell absorbers: A first-principles study

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Screened-exchange density functional theory description of the electronic structure and phase stability of the chalcopyrite materialsAgInSe2andAuInSe2

Cited by 12 publications

References 41 publications

First‐Principles Modeling of Point Defects and Complexes in Thin‐Film Solar‐Cell Absorber CuInSe2

First‐Principles Modeling of Point Defects and Complexes in Thin‐Film Solar‐Cell Absorber CuInSe2

Improved electronic structure prediction of chalcopyrite semiconductors from a semilocal density functional based on Pauli kinetic energy enhancement factor

Investigation of Ag(Ga,In)Se2 as thin-film solar cell absorbers: A first-principles study

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First‐Principles Modeling of Point Defects and Complexes in Thin‐Film Solar‐Cell Absorber CuInSe₂

First‐Principles Modeling of Point Defects and Complexes in Thin‐Film Solar‐Cell Absorber CuInSe₂