Physisorption of Water on Graphene: Subchemical Accuracy from Many-Body Electronic Structure Methods

Brandenburg, Jan Gerit; Zen, Andrea; Fitzner, Martin; Ramberger, Benjamin; Kresse, Georg; Tsatsoulis, Theodoros; Grüneis, Andreas; Michaelides, Angelos; Alfè, Dario

doi:10.1021/acs.jpclett.8b03679

Cited by 117 publications

(198 citation statements)

References 143 publications

(293 reference statements)

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“…Currently available QC approaches are based mostly on embedding, fragment models, the incremental technique or finite-cluster calculations (Voloshina et al, 2011;Libisch et al, 2012;Usvyat et al, 2012;Boese and Sauer, 2016;Kubas et al, 2016). Recently we have performed fully periodic calculations of adsorption energies for water on h−BN and graphene sheets, confirming the expected level of accuracy Brandenburg et al, 2019). Table 4 summarizes the results of the water adsorption energies and compares them to DMC findings that agree well.…”

Section: Paw-based Coupled Cluster Applicationssupporting

confidence: 54%

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Coupled Cluster Theory in Materials Science

2019

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The workhorse method of computational materials science is undeniably the density functional theory (DFT) in the Kohn-Sham framework of approximate exchange and correlation energy functionals. However, the need for highly accurate electronic structure theory calculations in materials science motivates the further development and exploration of alternative as well as complementary techniques. Among these alternative approaches, quantum chemical wavefunction based theories and in particular coupled cluster theory hold promise in filling the gap in the toolbox of computational materials scientists. Coupled cluster (CC) theory provides a compelling framework of approximate infinite-order perturbation theory, in the form of an exponential of cluster operators describing the true quantum many-body effects of the electronic wave function at a computational cost that, despite being significantly more expensive than DFT, scales polynomially with system size. The hierarchy of size-extensive approximate methods established in the framework of CC theory, achieves systematic improvability for many materials properties. This is in contrast to currently available density functionals that often suffer from uncontrolled approximations that limit the accuracy in the prediction of materials properties. In this tutorial-style review we will introduce basic concepts of coupled cluster theory and recent developments that increase its computational efficiency for calculations of molecules, solids and materials in general. We will touch upon the connection between coupled cluster theory and the random-phase approximation that is widely used in the field of solid-state physics. We will discuss various approaches to improve the computational performance without compromising on accuracy. These approaches include large-scale parallel design as well as techniques that reduce the pre-factor of the computational complexity. A central part of this article discusses the convergence of calculated properties to the thermodynamic limit, which is of significant importance for reliable predictions of materials properties and constitutes an additional challenge compared to calculations of large molecules. We mention technical aspects of computer code implementations of periodic coupled cluster theories in different numerical frameworks of the one-electron orbital basis; the projector-augmented-wave formalism using a plane wave basis set and the numeric atom-centered-orbital (NAO) with resolution-of-identity. We will discuss results and the possible scope of these implementations and how they can help advance the current state of the art in electronic structure theory calculations of materials.

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Section: Paw-based Coupled Cluster Applicationssupporting

confidence: 54%

“…The numbers in parenthesis have been obtained without finite size corrections. All values have been taken fromAl-Hamdani et al (2017),,and Brandenburg et al (2019).…”

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confidence: 99%

Coupled Cluster Theory in Materials Science

2019

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“…The reference values for water on benzene, coronene, and graphene with different orientations are taken from Ref. 57. The reference interaction energy between water and CNT where previously investigated in Ref.…”

Section: B Reference Interaction Energiesmentioning

confidence: 99%

Interaction between water and carbon nanostructures: How good are current density functional approximations?

Brandenburg

Zen

Michaelides

2019

The Journal of Chemical Physics

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Due to their current and future technological applications, including realisation of water filters and desalination membranes, water adsorption on graphitic sp 2 -bonded carbon is of overwhelming interest. However, these systems are notoriously challenging to model, even for electronic structure methods such as density functional theory (DFT), because of the crucial role played by London dispersion forces and non-covalent interactions in general. Recent efforts have established reference quality interactions of several carbon nanostructures interacting with water. Here, we compile a new benchmark set (dubbed WaC18), which includes a single water molecule interacting with a broad range of carbon structures, and various bulk (3D) and two dimensional (2D) ice polymorphs. The performance of 28 approaches, including semi-local exchange-correlation functionals, non-local (Fock) exchange contributions, and long-range van der Waals (vdW) treatments, are tested by computing the deviations from the reference interaction energies. The calculated mean absolute deviations on the WaC18 set depends crucially on the DFT approach, ranging from 135 meV for LDA to 12 meV for PBE0-D4. We find that modern vdW corrections to DFT significantly improve over their precursors. Within the 28 tested approaches, we identify the best performing within the functional classes of: generalized gradient approximated (GGA), meta-GGA, vdW-DF, and hybrid DF, which are BLYP-D4, TPSS-D4, rev-vdW-DF2, and PBE0-D4, respectively.

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“…44 and applied, e.g., for the phase diagram of ice 39 and for the binding energy curve of water on graphene. 35 While due to technical reasons it is currently not possible to run large scale computations of GWSE for molecules using VASP, we have computed GWSE for a single neon trimer at θ = 45 • and R = 3.0 Å to probe its effect for the systems considered in this work (see Table 7). For RPA(SCAN), the difference between GWSE and RSE corrections is on the same order of Table 5: Nonadditive energies for the challenging and easy subsets of the 3B-69 dataset.…”

Section: Low Dispersion Medium Dispersion High Dispersionmentioning

confidence: 99%

Random Phase Approximation Applied to Many-Body Noncovalent Systems

Modrzejewski

Yourdkhani

Klimeš

2019

J. Chem. Theory Comput.

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The random phase approximation (RPA) has received a considerable interest in the field of modeling systems where noncovalent interactions are important. Its advantages over widely used density functional theory (DFT) approximations are the exact treatment of exchange and the description of long-range correlation. In this work we address two open questions related to RPA. First, how accurately RPA describes nonadditive interactions encountered in many-body expansion of a binding energy. We consider three-body nonadditive energies in molecular and atomic clusters. Second, how does the accuracy of RPA depend on input provided by different DFT models, without resorting to selfconsistent RPA procedure which is currently impractical for calculations employing periodic boundary conditions. We find that RPA based on the SCAN0 and PBE0 models, i.e., hybrid DFT, achieves an overall accuracy between CCSD and MP3 on a dataset of molecular trimers of Řezáč et al. (J. Chem. Theory. Comput. 2015, 11, 3065) Finally, many-body expansion for molecular clusters and solids often leads to a large number of small contributions that need to be calculated with a high precision. We therefore present a cubic-scaling (or SCF-like) implementation of RPA in atomic basis set, which is designed for calculations with a high numerical precision. rors originating from the exchange functional are on the same order as the errors originating from the missing dispersion energy. [19][20][21] Approximate exchange functionals alone can lead to both strongly overestimated and underestimated noncovalent interactions. 22 For two body systems such issues tend to be masked by adjusting the equilibrium-and short-distance behavior of the dispersion correction. 19 However, the three-body exchange errors cannot be compensated in a similar way by adjusting the pairwise additive dispersion corrections. 19 Overall, the conclusion originating from the existing literature is that no existing semilocal functional can reliably account for many body effects. 21,23 Affordable schemes based on perturbation theory could offer higher and systematically improvable accuracy for calculations of condensed systems compared to standard DFT functionals. 21,[24][25][26][27] Of such schemes, the random phase approximation to the correlation energy (RPA) is promising as it is both compatible with the Hartree-Fock (HF) exchange and it contains terms describing higher-order (nonadditive) correlation effects. 28,29 RPA has been tested for interaction energies of dimers, 30-32 for adsorption, [33][34][35] or for molecular 36-39 and atomic solids 40 and interfaces. 41,42 For the cases involving noncovalent interactions, high accuracy has been achieved with addition of the singles corrections. 43,44 However, its accuracy for predicting nonadditive energies is unknown and this is one of our interests in this work. Moreover, most of the RPA calculations nowadays are performed non-self-consistently, using DFT orbitals and energies in the RPA energy expression. Here we obtain RPA results usi...

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Physisorption of Water on Graphene: Subchemical Accuracy from Many-Body Electronic Structure Methods

Cited by 117 publications

References 143 publications

Coupled Cluster Theory in Materials Science

Coupled Cluster Theory in Materials Science

Interaction between water and carbon nanostructures: How good are current density functional approximations?

Random Phase Approximation Applied to Many-Body Noncovalent Systems

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