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See detailPerformance of various density-functional approximations for cohesive properties of 64 bulk solids
Zhang, Guo-Xu; Reilly, Anthony; Tkatchenko, Alexandre UL et al

in New Journal of Physics (2018), 20

Accurate and careful benchmarking of different density-functional approximations (DFAs) represents an important source of information for understanding DFAs and how to improve them. In this work we have ... [more ▼]

Accurate and careful benchmarking of different density-functional approximations (DFAs) represents an important source of information for understanding DFAs and how to improve them. In this work we have studied the lattice constants, cohesive energies, and bulk moduli of 64 solids using six functionals, representing the local, semi-local, and hybrid DFAs on the first four rungs of Jacob’s ladder. The set of solids considered consists of ionic crystals, semiconductors, metals, and transition metal carbides and nitrides. To minimize numerical errors and to avoid making further approximations, the full-potential, all-electron FHI-aims code has been employed, and all the reported cohesive properties include contributions from zero-point vibrations. Our assessment demonstrates that current DFAs can predict cohesive properties with mean absolute relative errors of 0.6% for the lattice constant and6%for both the cohesive energy and the bulk modulus over the whole database of 64 solids. For semiconducting and insulating solids, the recently proposed SCAN meta-GGA functional represents a substantial improvement over the other functionals. However, when considering the different types of solids in the set, all of the employed functionals exhibit some variance in their performance. There are clear trends and relationships in the deviations of the cohesive properties, pointing to the need to consider, for example, long-range van der Waals (vdW) interactions. This point is also demonstrated by consistent improvements in predictions for cohesive properties of semiconductors when augmentingGGAand hybrid functionals with a screened Tkatchenko– Scheffler vdW energy term. [less ▲]

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See detailQuantitative Prediction of Optical Absorption in Molecular Solids from an Optimally Tuned Screened Range-Separated Hybrid Functional
Manna, Arun; Refaely-Abramson, Sivan; Reilly, Anthony et al

in Journal of Chemical Theory and Computation (2018), 14

We show that fundamental gaps and optical spectra of molecular solids can be predicted quantitatively and nonempirically within the framework of time-dependent density functional theory (TDDFT) using the ... [more ▼]

We show that fundamental gaps and optical spectra of molecular solids can be predicted quantitatively and nonempirically within the framework of time-dependent density functional theory (TDDFT) using the recently developed optimally tuned screened range-separated hybrid (OT-SRSH) functional approach. In this scheme, the electronic structure of the gas-phase molecule is determined by optimal tuning of the range-separation parameter in a range-separated hybrid functional. Screening and polarization in the solid state are taken into account by adding long-range dielectric screening to the functional form, with the modified functional used to perform self-consistent periodic boundary calculations for the crystalline solid. We provide a comprehensive benchmark for the accuracy of our approach by considering the X23 set of molecular solids and comparing results obtained from TDDFT with those obtained from many-body perturbation theory in the GW-BSE approximation. We additionally compare results obtained from dielectric screening computed within the random-phase approximation to those obtained from the computationally more efficient many-body dispersion approach and find that this influences the fundamental gap but has little effect on the optical spectra. Our approach is therefore robust and can be used for studies of molecular solids that are typically beyond the reach of computationally more intensive methods. [less ▲]

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See detailTerahertz spectroscopy of 2,4,6-trinitrotoluene molecular solids from first principles
Azuri, Ido; Hirsch, Anna; Reilly, Anthony et al

in Beilstein Journal of Organic Chemistry (2018), 14

We present a computational analysis of the terahertz spectra of the monoclinic and the orthorhombic polymorphs of 2,4,6-trinitrotoluene. Very good agreement with experimental data is found when using ... [more ▼]

We present a computational analysis of the terahertz spectra of the monoclinic and the orthorhombic polymorphs of 2,4,6-trinitrotoluene. Very good agreement with experimental data is found when using density functional theory that includes Tkatchenko–Scheffler pair-wise dispersion interactions. Furthermore, we show that for these polymorphs the theoretical results are only weakly affected by many-body dispersion contributions. The absence of dispersion interactions, however, causes sizable shifts in vibrational frequencies and directly affects the spatial character of the vibrational modes. Mode assignment allows for a distinction between the contributions of the monoclinic and orthorhombic polymorphs and shows that modes in the range from 0 to ca. 3.3 THz comprise both inter- and intramolecular vibrations, with the former dominating below ca. 1.5 THz. We also find that intramolecular contributions primarily involve the nitro and methyl groups. Finally, we present a prediction for the terahertz spectrum of 1,3,5-trinitrobenzene, showing that a modest chemical change leads to a markedly different terahertz spectrum. [less ▲]

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