Meta-generalized Gradient Approximation Research Articles

Dispersion corrected r2SCAN based global hybrid functionals: r2SCANh, r2SCAN0, and r2SCAN50.

The regularized and restored semilocal meta-generalized gradient approximation (meta-GGA) exchange-correlation functional r2SCAN [Furness et al., J. Phys. Chem. Lett. 11, 8208-8215 (2020)] is used to create three global hybrid functionals with varying admixtures of Hartree-Fock "exact" exchange (HFX). The resulting functionals r2SCANh (10% HFX), r2SCAN0 (25% HFX), and r2SCAN50 (50% HFX) are combined with the semi-classical D4 London dispersion correction. The new functionals are assessed for the calculation of molecular geometries, main-group, and metalorganic thermochemistry at 26 comprehensive benchmark sets. These include the extensive GMTKN55 database, ROST61, and IONPI19 sets. It is shown that a moderate admixture of HFX leads to relative improvements of the mean absolute deviations for thermochemistry of 11% (r2SCANh-D4), 16% (r2SCAN0-D4), and 1% (r2SCAN50-D4) compared to the parental semi-local meta-GGA. For organometallic reaction energies and barriers, r2SCAN0-D4 yields an even larger mean improvement of 35%. The computation of structural parameters (geometry optimization) does not systematically profit from the HFX admixture. Overall, the best variant r2SCAN0-D4 performs well for both main-group and organometallic thermochemistry and is better or on par with well-established global hybrid functionals, such as PW6B95-D4 or PBE0-D4. Regarding systems prone to self-interaction errors (SIE4x4), r2SCAN0-D4 shows reasonable performance, reaching the quality of the range-separated ωB97X-V functional. Accordingly, r2SCAN0-D4 in combination with a sufficiently converged basis set [def2-QZVP(P)] represents a robust and reliable choice for general use in the calculation of thermochemical properties of both main-group and organometallic chemistry.

Meta-GGA exchange-correlation free energy density functional to increase the accuracy of warm dense matter simulations

We discuss strategies for thermalization of the ground-state meta-generalized gradient approximation (meta-GGA) exchange-correlation (XC) functionals. A simple but accurate scheme is implemented via universal additive thermal correction to XC using a perturbativelike self-consistent approach. The additive correction with explicit temperature dependence is applied to the ground-state deorbitalized, strongly constrained, and appropriately normed (SCAN-L) meta-GGA XC leading to a thermal XC functional denoted here as T-SCAN-L. The thermal T-SCAN-L meta-GGA functional shows significant improvement in density functional theory calculation accuracy for warm dense matter by a factor of 3 to 10, achieving an accuracy of total pressure between a few tenths and $\ensuremath{\sim}1$% when compared to traditional XC functionals, as demonstrated by the comparison to path-integral Monte Carlo simulations for helium equation of state. The T-SCAN-L calculations of dc conductivity of warm dense aluminum also give better agreement with experiments over other XC functionals such as PBE and SCAN-L.

Sensitivity of the electronic and magnetic structures of cuprate superconductors to density functional approximations

We discuss the crystal, electronic, and magnetic structures of La2−xSrxCuO4 (LSCO) for x = 0.0 and x = 0.25 employing 13 density functional approximations, representing the local, semi-local, and hybrid exchange-correlation approximations within the Perdew–Schmidt hierarchy. The meta-generalized gradient approximation (meta-GGA) class of functionals is found to perform well in capturing the key properties of LSCO, a prototypical high-temperature cuprate superconductor. In contrast, the localspin-density approximation, GGA, and the hybrid density functional fail to capture the metal-insulator transition under doping.

Bending as a control knob for the electronic and optical properties of phosphorene nanoribbons

We have assessed mechanical bending as a powerful controlling tool for the electronic structure and optical properties of phosphorene nanoribbons. We use state-of-the-art density functional approximations in our work. The overall performance of the recently developed meta-generalized gradient approximation (meta-GGA) mTASK [Phys. Rev. Materials 5, 063803 (2021)] functional establishes the method as a useful alternative to the screened hybrid HSE06 for better band gaps of phosphorene nanoribbons. We present a detailed analysis to interpret the optical absorption of bent phosphorene nanoribbons using the GW-Bethe-Salpeter approximation. We demonstrate the important role of the unoccupied in-gap state and conclude that this in-gap state in armchair nanoribbons introduced by bending can significantly affect the properties of low-energy excitons and add some useful opportunities for applications in optoelectronic devices.

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

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) (2019 Phys. Rev. B 100 155140) 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.

Adsorption performance of TM doped (TM = Fe, Ni, Cr and Zn) silicon carbide nanotubes towards formaldehyde: a DFT-M06-L study

In this work, the adsorption of formaldehyde (H2CO) on the surface of transition metal-doped silicon carbide nanotubes (TM-SiCNTs; TM = Fe, Ni, Cr and Zn) were scrutinised by using M06-L meta-generalised gradient approximation (m-GGA) exchange–correlation functional. Two types of TMSi–SiCNTs and TMC–SiCNTs doped nanostructures were found on the potential energy surfaces. The obtained results indicate that the TMSi–SiCNTs are more stable than TMC–SiCNTs. The adsorption energies of H2CO on the TM doped SiCNTs are computed to be in the range of −0.55 to −2.52 eV. The sequence of H2CO adsorption energies on the metal-doped silicon carbide nanotubes are H2CO-CrC-SiCNT > H2CO-FeC-SiCNT > H2CO-FeSi-SiCNT > H2CO-CrSi-SiCNT > H2CO-NiC-SiCNT > H2CO-ZnC-SiCNT > H2CO-NiSi-SiCNT > H2CO-ZnSi-SiCNT. In comparison with the pure SiCNT, the HOMO–LUMO gap decreases and electrical conductance increases. The change in the HOMO–LUMO gap of NiC-SiCNT is predicted to be greater than those of others. Therefore, the NiC-SiCNT is predicted to be more sensitive than other metal-doped NTs to H2CO gas. These results give new insights into the applications of TM-SiCNTs materials in H2CO gas sensing.

Performances of different DFT functionals to calculate the anodic limit of fluorinated sulphonyl-imide anions for lithium cells

In this paper we investigated the calculation of the anodic limit of two anions of ionic liquids, largely used as electrolyte of lithium batteries. Starting from a model based on calculations performed on single ions at the MP2 level of theory, we showed that the matching between calculation and experiments decreases while using more expanded basis set with respect to 6-31G**, possibly because of the destabilization of the neutral species when larger basis sets are considered. Additionally, in order to decrease the computational time, the performances for the calculation of the anodic limit obtained by means of a series of DFT functionals with increasing level of complexity (from the Generalized Gradient Approximation to the Range Separated Hybrid meta-Generalized Gradient Approximation) were compared. Overall, the best performing functionals are BMK, ωB97M-V and MN12-SX, while acceptable results can be obtained by M06-2X, M11, M08-HX and M11-L. Some less computationally expensive functionals, like CAM-B3LYP and ωB97X-D, also provide reasonable values of the anodic limit.

Improved first-principles equation-of-state table of deuterium for high-energy-density applications

We present a first-principles equation-of-state (EOS) table of deuterium aimed at improving the previously established first-principles equation-of-state table (FPEOS) [S. X. Hu et al., Phys. Rev. B 84, 224109 (2011); S. X. Hu et al., Phys. Plasmas 22, 056304 (2015)]. The EOS table presented here, referred to as iFPEOS, introduces (1) a universal density functional theory (DFT) treatment of all density and temperature conditions, (2) a fully consistent treatment of exchange-correlation (XC) thermal effects across the entire range of temperatures covered, and (3) quantum treatment of ions. Based on ab initio molecular dynamics driven by thermal density functional theory, iFPEOS includes density points in the range $1\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}3}\ensuremath{\le}\ensuremath{\rho}\ensuremath{\le}1.6\ifmmode\times\else\texttimes\fi{}{10}^{3}$ $\mathrm{g}/{\mathrm{cm}}^{3}$ and temperature points in the range 800 K $\ensuremath{\le}T\ensuremath{\le}256$ MK, thus covering the challenging warm dense matter (WDM) regime. For an improved description of the electronic structure, iFPEOS employs an advanced free-energy XC density functional with explicit temperature dependence, which is at the metageneralized gradient approximation level of DFT. We use the latest orbital-free free-energy density functional for the high-temperature regime where it shows excellent agreement with standard Mermin-Kohn-Sham DFT. For quantum treatment of ions we use path-integral molecular dynamics in order to take into account nuclear quantum effects. Results are compared to other EOS models and most recent experimental measurements of deuterium properties such as the molecular-to-atomic fluid transition, the principal and reshock Hugoniot, and sound speed. We find that iFPEOS provides an improved agreement with experimental data compared to other first-principles EOS models in the WDM regime for pressures up to 200 GPa and temperatures up to $60\phantom{\rule{0.16em}{0ex}}000$ K. For higher pressures and temperatures, however, iFPEOS is in agreement with other models in predicting lower compressibility and higher sound speed along the Hugoniot, compared to experiment.

Investigation of structural, morphological, and optoelectronic properties of Ga-doped TiO2 nanoparticles for electron transport layer in solar cell applications: An experimental and theoretical study

In the current work, the sol-gel synthesis method was used to synthesize both undoped and gallium (1%-Ga) doped TiO2 nanoparticles. The as-deposited materials were calcined at 400–500 °C with a temperature variation rate of 5 °C per minute. The crystallographic properties of the semiconductor materials were determined from X-ray diffraction (XRD) which showed the formation of anatase TiO2. The average crystallite sizes, determined from the widths of the XRD reflections, were 11 and 4 nm for undoped and Ga-doped TiO2, respectively. The materials were further studied by density functional theory with meta-generalized gradient approximation exchange–correlation functional. Supercell systems consisting of 24 and 48 atoms were created to form 12.5% and 6.25% Ga dopant substitution, respectively. These structures were optimized to obtain the ground state properties. Transmission electron microscopy showed polycrystalline, spherical powders, with grain sizes comparable to those found using XRD. The surface morphology of the doped TiO2 obtained from scanning electron microscopy showed an improved surface structure compared to pristine TiO2. Moreover, the electronic states of the materials were investigated using X-ray photoelectron spectroscopy. Energy dispersive X-ray spectroscopy verified the elemental composition of titanium, oxygen, and Ga present in the nanoparticles. The surface chemical bonds were analyzed by Fourier-transform infrared spectroscopy. Ultraviolet diffused reflectance spectra analysis was used to examine their optical properties. The experimentally obtained bandgaps of pristine and 1% Ga-doped TiO2 nanoparticles were 2.9 and 3.09 eV, respectively. The optical properties were further analyzed by computing the band structures and density of states using density functional theory. Similar to the experimental results, these electronic structures showed an increase in bandgap after 6.25% Ga incorporation. However, with 12.5% doping, there was a decrement in the bandgap. The analysis showed that, with an appropriate amount of substitution, Ga-doped TiO2 semiconductor material can be used in the electron transport layer and many other fields of photoelectric cells.

Defect levels from SCAN and MBJ meta-GGA exchange-correlation potentials

For more than a decade the HSE06 hybrid exchange-correlation functional developed by Heyd, Scuseria and Ernzerhof has provided a tool for reliable defect level calculations in density functional theory for which postprocessing tools are not necessary, in contrast to previous calculations using semilocal density functionals. One of the main reasons for its reliability is the high precision of HSE06 for band gap calculations. Recently, other functionals from the meta-generalized gradient approximation (meta-GGA) class have been used extensively to calculate the electronic properties of solids. In particular, band gaps can be accurately evaluated with the modified Becke-Johnson (MBJ) potential, and relaxed atomic structures close to experimental findings can be obtained with the strongly constrained and appropriately normed (SCAN) exchange-correlation functional. Both approaches are computationally cheaper than HSE06, and we consider here their performance for defect level calculations. We compare results for the $\ensuremath{\epsilon}(+/0)$ transition levels of seven donors and $\ensuremath{\epsilon}(0/\ensuremath{-})$ transition levels of four acceptors in group IV semiconductors. We conclude that in certain situations where HSE06 cannot be applied because of excessive computational costs, SCAN and MBJ might provide a good alternative.

Hydration structures of barium ions: Ab initio molecular dynamics simulations using the SCAN meta-GGA density functional and EXAFS spectroscopy studies

Hydration structures of barium ion (Ba2+) were studied by ab initio molecular dynamics using the strongly constrained and appropriately normed (SCAN) meta-generalized gradient approximation (GGA) exchange-correlation (XC) functional and extended X-ray absorption fine structure spectroscopy, which showed consistent results for the static properties. The result obtained with SCAN was compared with these with the Perdew–Burke–Ernzerhof (PBE) and Becke–Lee–Yang–Parr (BLYP) GGA XC functionals and the functionals with the Grimme’s dispersion correction (PBE-D3 and BLYP-D3). The comparison revealed the importance of the dispersion interaction for the static and dynamic properties of the Ba2+ hydration structures.

The Vibrational and Thermodynamic Properties of CsPbI3 Polymorphs: An Improved Description Based on the SCAN meta-GGA Functional.

We report the vibrational and thermodynamic properties of four known CsPbI3 polymorphs in the framework of the density functional theory. We compare the recently introduced strongly constrained and appropriately normed (SCAN) meta-generalized gradient approximation (meta-GGA) with the local density approximation (LDA). We found that the SCAN, compared to the LDA, could explain discrepancies between theoretical and experimental results. Evaluating the Helmholtz free energy as a function of temperature, we found that within the SCAN (a) all polymorphs had negative formation enthalpies at the room temperature and (b) CsPbI3 underwent the phase transition from the δ- to α-phase at 480 K. This is not true for the LDA. In contrast to the previous reports based on the LDA, we did not find the ferroelectric instability in the phonon spectra of the cubic and tetragonal phases at the meta-GGA level. This result agrees with the lack of observation of the ferroelectricity in CsPbI3.

Improving the applicability of the Pauli kinetic energy density based semilocal functional for solids

The Pauli kinetic energy enhancement factor α = (τ − τ W )/τ unif is an important density ingredient, used to construct many meta-generalized gradient approximations (meta-GGA) exchange–correlation (XC) energy functionals, including the very successful strongly constrained and appropriately normed (SCAN) semilocal functional. Another meta-GGA functional, known as MGGAC (2019 Phys. Rev. B 100 155140), is also proposed in recent time depending only on the α ingredient and based on the generalization of the Becke–Roussel approach with the cuspless hydrogen exchange hole density. The MGGAC functional is proved to be a very useful and competitive meta-GGA semilocal functional for electronic structure properties of solids and molecules. Based on the successful implication of the ingredient α, which is also useful to construct the one-electron self-interaction free correlation energy functional, here we propose revised correlation energy for MGGAC exchange functional which is more accurate and robust, especially for the high and low-density limits of the uniform density scaling. The present XC functional, named as revised MGGAC (rMGGAC), shows an impressive improvement for the structural and energetic properties of solids compared to its previous version. Moreover, the assessment of the present constructed functional shows to be quite useful in solid-state physics in terms of addressing several current challenging solid-state problems.

Theoretical Basis of Quantum-Mechanical Modeling of Functional Nanostructures

The paper presents an analytical review of theoretical methods for modeling functional nanostructures. The main evolutionary changes in the approaches of quantum-mechanical modeling are described. The foundations of the first-principal theory are considered, including the stationery and time-dependent Schrödinger equations, wave functions, the form of writing energy operators, and the principles of solving equations. The idea and specifics of describing the motion and interaction of nuclei and electrons in the framework of the theory of the electron density functional are presented. Common approximations and approaches in the methods of quantum mechanics are presented, including the Born–Oppenheimer approximation, the Hartree–Fock approximation, the Thomas–Fermi theory, the Hohenberg–Kohn theorems, and the Kohn–Sham formalism. Various options for describing the exchange–correlation energy in the theory of the electron density functional are considered, such as the local density approximation, generalized and meta-generalized gradient approximations, and hybridization of the generalized gradient method. The development of methods of quantum mechanics to quantum molecular dynamics or the dynamics of Car–Parrinello is shown. The basic idea of combining classical molecular modeling with calculations of the electronic structure, which is reflected in the potentials of the embedded atom, is described.

Efficient Band Structure Calculation of Two-Dimensional Materials from Semilocal Density Functionals.

The experimental and theoretical realization of two-dimensional (2D) materials is of utmost importance in semiconducting applications. Computational modeling of these systems with satisfactory accuracy and computational efficiency is only feasible with semilocal density functional theory methods. In the search for the most useful method in predicting the band gap of 2D materials, we assess the accuracy of recently developed semilocal exchange–correlation (XC) energy functionals and potentials. Though the explicit forms of exchange–correlation (XC) potentials are very effective against XC energy functionals for the band gap of bulk solids, their performance needs to be investigated for 2D materials. In particular, the LMBJ [J. Chem. Theory Comput.2020, 16, 265432097004] and GLLB-SC [Phys. Rev. B82, 2010, 115106] potentials are considered for their dominance in bulk band gap calculation. The performance of recently developed meta generalized gradient approximations, like TASK [Phys. Rev. Res.1, 2019, 033082] and MGGAC [Phys. Rev. B. 100, 2019, 155140], is also assessed. We find that the LMBJ potential constructed for 2D materials is not as successful as its parent functional, i.e., MBJ [Phys. Rev. Lett.102, 2009, 22640119658882] in bulk solids. Due to a contribution from the derivative discontinuity, the band gaps obtained with GLLB-SC are in a certain number of cases, albeit not systematically, larger than those obtained with other methods, which leads to better agreement with the quasi-particle band gap obtained from the GW method. The band gaps obtained with TASK and MGGAC can also be quite accurate.

Performance of Made Simple Meta-GGA Functionals with rVV10 Nonlocal Correlation for H2 + Cu(111), D2 + Ag(111), H2 + Au(111), and D2 + Pt(111).

Accurately modeling heterogeneous catalysis requires accurate descriptions of rate-controlling elementary reactions of molecules on metal surfaces, but standard density functionals (DFs) are not accurate enough for this. The problem can be solved with the specific reaction parameter approach to density functional theory (SRP-DFT), but the transferability of SRP DFs among chemically related systems is limited. We combine the MS-PBEl, MS-B86bl, and MS-RPBEl semilocal made simple (MS) meta-generalized gradient approximation (GGA) (mGGA) DFs with rVV10 nonlocal correlation, and we evaluate their performance for the hydrogen (H2) + Cu(111), deuterium (D2) + Ag(111), H2 + Au(111), and D2 + Pt(111) gas-surface systems. The three MS mGGA DFs that have been combined with rVV10 nonlocal correlation were not fitted to reproduce particular experiments, nor has the b parameter present in rVV10 been reoptimized. Of the three DFs obtained the MS-PBEl-rVV10 DF yields an excellent description of van der Waals well geometries. The three original MS mGGA DFs gave a highly accurate description of the metals, which was comparable in quality to that obtained with the PBEsol DF. Here, we find that combining the three original MS mGGA DFs with rVV10 nonlocal correlation comes at the cost of a slightly less accurate description of the metal. However, the description of the metal obtained in this way is still better than the descriptions obtained with SRP DFs specifically optimized for individual systems. Using the Born–Oppenheimer static surface (BOSS) model, simulations of molecular beam dissociative chemisorption experiments yield chemical accuracy for the D2 + Ag(111) and D2 + Pt(111) systems. A comparison between calculated and measured E1/2(ν, J) parameters describing associative desorption suggests chemical accuracy for the associative desorption of H2 from Au(111) as well. Our results suggest that ascending Jacob’s ladder to the mGGA rung yields increasingly more accurate results for gas-surface reactions of H2 (D2) interacting with late transition metals.

Coverage-dependent adsorption of small gas molecules on black phosphorene: a DFT study

Using Density Functional Theory (DFT), we perform a detailed computational study to explore the adsorption behaviors of NH3, NO, NO2, CO and CO2 gas molecules on a black phosphorene surface at several coverages. Van der Waals (vdW) interactions were taken into account within the optB88-vdW functional. In addition, a comparison with the strongly-constrained and appropriately-normed (SCAN) meta-generalized gradient approximation (meta-GGA) is discussed. Our calculations show that all molecules adsorb on the surface of black phosphorene with different favorable adsorption sites, depending on the molecule's geometry and orientation. Alongside the adsorption energies, other properties are presented including the adsorption distances and charge transfers. At high coverages, the adsorption energies per molecule show that the functionals start to behave differently as the coverage rate increases. The significant charge transfer between NO and NO2 molecules and black phosphorene suggests its potential integration towards efficient nitrogen-oxide detectors.

Accurate and Numerically Efficient r 2 SCAN Meta-Generalized Gradient Approximation

The recently proposed rSCAN functional [J. Chem. Phys. 150, 161101 (2019)] is a regularized form of the SCAN functional [Phys. Rev. Lett. 115, 036402 (2015)] that improves SCAN's numerical performance at the expense of breaking constraints known from the exact exchange-correlation functional. We construct a new meta-generalized gradient approximation by restoring exact constraint adherence to rSCAN. The resulting functional maintains rSCAN's numerical performance while restoring the transferable accuracy of SCAN.

Effect of the Current Dependence of Tau-Dependent Exchange-Correlation Functionals on Nuclear Shielding Calculations.

Exchange-correlation functionals that depend on the local kinetic energy τ are widely used in many fields. This includes meta-generalized gradient approximation (GGA) functionals and their global hybrid versions as well as local hybrid functionals with τ-dependent local mixing functions to determine position-dependent exact-exchange admixture. Under the influence of an external magnetic field, τ becomes dependent on the gauge of the magnetic vector potential and should thus be extended to a gauge-invariant formulation. The currently most widely used extension for nuclear shielding calculations is that suggested by Maximoff and Scuseria (Maximoff, S. N.; Scuseria, G. E. Chem. Phys. Lett. 2004, 390, 408). Using the recent first implementation of local hybrids in this framework, we have found unphysical paramagnetic contributions, which are most clearly identified for atoms but are also present in molecules. These τMS artifacts are small for the TPSS or TPSSh functionals, significantly deshielding in the case of nonhydrogen nuclei for the M06-L and M06 functionals and significantly shielding in those cases for the first-generation τ-dependent local hybrids LH07t-SVWN and LH12ct-SsifPW92. We have therefore implemented an extension of a linear-response nuclear shielding code to the proper current-density functional version of τ suggested by Dobson (Dobson, J. F. J. Chem. Phys. 1993, 98, 8870). Using τD eliminates the gauge dependence as well as the unphysical contributions introduced by τMS. A first evaluation of this implementation for a set of main-group nuclear shieldings against CCSD(T) benchmark data indicates rather small effects for the TPSS and TPSSh functionals but significant changes for the other functionals studied: the previously observed remarkable performance of the highly parameterized meta-GGA functional M06-L is found to be the result of error compensation with the lack of an explicit current dependence. Results for the M06 functional are improved somewhat but are still overall of relatively low accuracy. In contrast, too low proton shieldings found recently for τ-dependent local hybrids are improved significantly within the τD current-density functional framework while preserving the outstanding performance of these functionals for other nuclei.

R2SCAN-D4: Dispersion corrected meta-generalized gradient approximation for general chemical applications.

We combine a regularized variant of the strongly constrained and appropriately normed semilocal density functional [J. Sun, A. Ruzsinszky, and J. P. Perdew, Phys. Rev. Lett. 115, 036402 (2015)] with the latest generation semi-classical London dispersion correction. The resulting density functional approximation r2SCAN-D4 has the speed of generalized gradient approximations while approaching the accuracy of hybrid functionals for general chemical applications. We demonstrate its numerical robustness in real-life settings and benchmark molecular geometries, general main group and organo-metallic thermochemistry, and non-covalent interactions in supramolecular complexes and molecular crystals. Main group and transition metal bond lengths have errors of just 0.8%, which is competitive with hybrid functionals for main group molecules and outperforms them for transition metal complexes. The weighted mean absolute deviation (WTMAD2) on the large GMTKN55 database of chemical properties is exceptionally small at 7.5 kcal/mol. This also holds for metal organic reactions with an MAD of 3.3 kcal/mol. The versatile applicability to organic and metal-organic systems transfers to condensed systems, where lattice energies of molecular crystals are within the chemical accuracy (errors <1 kcal/mol).