From ultrasoft pseudopotentials to the projector augmented-wave method
TL;DR: In this paper, the formal relationship between US Vanderbilt-type pseudopotentials and Blochl's projector augmented wave (PAW) method is derived and the Hamilton operator, the forces, and the stress tensor are derived for this modified PAW functional.
Abstract: The formal relationship between ultrasoft (US) Vanderbilt-type pseudopotentials and Bl\"ochl's projector augmented wave (PAW) method is derived. It is shown that the total energy functional for US pseudopotentials can be obtained by linearization of two terms in a slightly modified PAW total energy functional. The Hamilton operator, the forces, and the stress tensor are derived for this modified PAW functional. A simple way to implement the PAW method in existing plane-wave codes supporting US pseudopotentials is pointed out. In addition, critical tests are presented to compare the accuracy and efficiency of the PAW and the US pseudopotential method with relaxed core all electron methods. These tests include small molecules $({\mathrm{H}}_{2}{,\mathrm{}\mathrm{H}}_{2}{\mathrm{O},\mathrm{}\mathrm{Li}}_{2}{,\mathrm{}\mathrm{N}}_{2}{,\mathrm{}\mathrm{F}}_{2}{,\mathrm{}\mathrm{BF}}_{3}{,\mathrm{}\mathrm{SiF}}_{4})$ and several bulk systems (diamond, Si, V, Li, Ca, ${\mathrm{CaF}}_{2},$ Fe, Co, Ni). Particular attention is paid to the bulk properties and magnetic energies of Fe, Co, and Ni.
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TL;DR: In this article, the authors show that self-interaction error and the neglect of spin-orbit coupling in many previous DFT calculations resulted in incorrect positions of valence and conduction band edges, although their difference is the band gap.
Abstract: Native point defects play an important role in carrier transport properties of CH3NH3PbI3. However, the nature of many important defects remains controversial due partly to the conflicting results reported by recent density functional theory (DFT) calculations. In this Letter, we show that self-interaction error and the neglect of spin–orbit coupling (SOC) in many previous DFT calculations resulted in incorrect positions of valence and conduction band edges, although their difference, which is the band gap, is in good agreement with the experimental value. This problem has led to incorrect predictions of defect-level positions. Hybrid density functional calculations, which partially correct the self-interaction error and include the SOC, show that, among native point defects (including vacancies, interstitials, and antisites), only the iodine vacancy and its complexes induce deep electron and hole trapping levels inside of the band gap, acting as nonradiative recombination centers.
313 citations
TL;DR: The hybrid PBE0 functional appears as a good compromise to obtain an accurate description of both structural and electronic properties of solids.
Abstract: The two polymorphs of TiO2, rutile and anatase, have been investigated at the ab initio level using different Hamiltonians with all-electron Gaussian and projector augmented plane wave basis sets. Their equilibrium lattice parameters, relative stabilities, binding energies, and band structures have been evaluated. The calculations have been performed at the Hartree-Fock, density functional theory (DFT), and hybrid (B3LYP and PBE0) levels. As regards DFT, the local density and generalized gradient (PBE) approximations have been used. Our results show an excellent agreement with the experimental band structures and binding energies for the B3LYP and PBE0 functionals, while the best structural descriptions are obtained at the PBE0 level. However, no matter which Hamiltonian and method are used, anatase is found more stable than rutile, in contrast with recent experimental reports, although the relative stabilities of the two phases are very close to each other. Nevertheless, based on the overall results, the hybrid PBE0 functional appears as a good compromise to obtain an accurate description of both structural and electronic properties of solids.
313 citations
TL;DR: Li et al. as discussed by the authors used an organometallic compound, ferrocenyl-bis-thiophene-2-carboxylate (FcTc2), to stabilize a multication perovskite layer of an inverted PSC.
Abstract: Further enhancing the performance and stability of inverted perovskite solar cells (PSCs) is crucial for their commercialization. We report that the functionalization of multication and halide perovskite interfaces with an organometallic compound, ferrocenyl-bis-thiophene-2-carboxylate (FcTc2), simultaneously enhanced the efficiency and stability of inverted PSCs. The resultant devices achieved a power conversion efficiency of 25.0% and maintained >98% of their initial efficiency after continuously operating at the maximum power point for 1500 hours under simulated AM1.5 illumination. Moreover, the FcTc2-functionalized devices passed the international standards for mature photovoltaics (IEC61215:2016) and have exhibited high stability under the damp heat test (85°C and 85% relative humidity). Description Organometallics stabilizing perovskites Perovskite solar cells with inverted (p-i-n) structure can have greater stability and lifetimes than conventional n-i-p structures but usually have somewhat lower power conversion efficiencies (PCEs). Li et al. report that an organometallic compound, ferrocenyl-bis-thiophene-2-carboxylate, can stabilize a multication perovskite layer of an inverted perovskite solar cells. After 1500 hours of maximum power point operation, 98% of the 25.0% PCE was maintained. The solar cell also exhibited high stability in damp heat tests. —PDS Functionalizing interfaces with an organometallic compound created an efficient and stable inverted perovskite solar cell.
313 citations
TL;DR: High-entropy alloys are a new class of materials that have been shown to be strong, ductile, and corrosion-resistant as mentioned in this paper, and have been systematically isolated using density-functional theory.
Abstract: High-entropy alloys are a new class of materials that have been shown to be strong, ductile, and corrosion-resistant. Ensembles of viable alloys are systematically isolated using density-functional theory.
313 citations
Cites methods from "From ultrasoft pseudopotentials to ..."
...To test this hypothesis, we perform DFT calculations [37,38] of the ΔHf for supercell models of the disordered phase....
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TL;DR: In this paper, the electronic properties of graphene upon water adsorption were investigated and the influence of the SiO2 substrate in this context using density functional calculations, and it was shown that H2O adsorbates can shift the substrate impurity bands and change their hybridization with the graphene bands.
Abstract: We investigate the electronic properties of graphene upon water adsorption and study the influence of the SiO2 substrate in this context using density functional calculations. Perfect suspended graphene is rather insensitive to H2O adsorbates, as doping requires highly oriented H2O clusters. For graphene on a defective SiO2 substrate, we find a strongly different behavior: H2O adsorbates can shift the substrate’s impurity bands and change their hybridization with the graphene bands. In this way, H2O can lead to doping of graphene for much lower adsorbate concentrations than for free hanged graphene. The effect depends strongly on the microscopic substrate properties.
312 citations
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Book•
31 Dec 1993
TL;DR: The linearized augmented planewave (LAPW) method has emerged as the standard by which density functional calculations for transition metal and rare-earth containing materials are judged.
Abstract: With its extreme accuracy and reasonable computational efficiency, the linearized augmented planewave (LAPW) method has emerged as the standard by which density functional calculations for transition metal and rare-earth containing materials are judged. This volume presents a thorough and self-conta
1,150 citations