Properties of the water to boron nitride interaction: from zero to two dimensions with benchmark accuracy

Abstract

Molecular adsorption on surfaces plays an important part in catalysis, corrosion, desalination, and various other processes that are relevant to industry and in nature. As a complement to experiments, accurate adsorption energies can be obtained using various sophisticated electronic structure methods that can now be applied to periodic systems. The adsorption energy of water on boron nitride substrates, going from zero to 2-dimensional periodicity, is particularly interesting as it calls for an accurate treatment of polarizable electrostatics and dispersion interactions, as well as posing a practical challenge to experiments and electronic structure methods. Here, we present reference adsorption energies, static polarizabilities, and dynamic polarizabilities, for water on BN substrates of varying size and dimension. Adsorption energies are computed with coupled cluster theory, fixed-node quantum Monte Carlo (FNQMC), the random phase approximation (RPA), and second order Møller-Plesset (MP2) theory. These explicitly correlated methods are found to agree in molecular as well as periodic systems. The best estimate of the water/h-BN adsorption energy is $-107\pm 7$ meV from FNQMC. In addition, the water adsorption energy on the BN substrates could be expected to grow monotonically with the size of the substrate due to increased dispersion interactions but interestingly, this is not the case here. This peculiar finding is explained using the static polarizabilities and molecular dispersion coefficients of the systems, as computed from time-dependent density functional theory (DFT). Dynamic as well as static polarizabilities are found to be highly anisotropic in these systems. In addition, the many-body dispersion method in DFT emerges as a particularly useful estimation of finite size effects for other expensive, many-body wavefunction based methods.

References in corpus (39)

• Van der Waals density functionals applied to solids
• Long-range correlation energy calculated from coupled atomic response functions
• Continuum variational and diffusion quantum Monte Carlo calculations
• Hydrogen bonds and van der Waals forces in ice at ambient and high pressures
• The Finite Size Error in Many-body Simulations with long-Ranged Interactions
• Finite-size errors in continuum quantum Monte Carlo calculations
• Beyond the Random Phase Approximation for the Electron Correlation Energy: The Importance of Single Excitations
• On the physisorption of water on graphene: a CCSD(T) study
• Predictive GW calculations using plane waves and pseudopotentials
• Benchmark tests of a strongly constrained semilocal functional with a long-range dispersion correction
• Smooth relativistic Hartree-Fock pseudopotentials for H to Ba and Lu to Hg
• Interatomic Methods for the Dispersion Energy Derived from the Adiabatic Connection Fluctuation-Dissipation Theorem
• Norm-conserving Hartree-Fock pseudopotentials and their asymptotic behavior
• An efficient localized basis set for quantum Monte Carlo calculations on condensed matter
• Size-consistent variational approaches to non-local pseudopotentials: standard and lattice regularized diffusion Monte Carlo methods revisited
• On the Accuracy of van der Waals Inclusive Density-Functional Theory Exchange-Correlation Functionals for Ice at Ambient and High Pressures
• Finite-size correction in many-body electronic structure calculations
• Theory of Finite Size Effects for Electronic Quantum Monte Carlo Calculations of Liquids and Solids
• Diffusion Monte Carlo with lattice regularization
• Green Function Monte Carlo with Stochastic Reconfiguration: an effective remedy for the sign problem disease
• Finite size errors in quantum many-body simulations of extended systems
• Boosting the accuracy and speed of quantum Monte Carlo: size-consistency and time-step
• Water on hexagonal boron nitride from diffusion Monte Carlo
• Ab-initio molecular dynamics simulation of liquid water by Quantum Monte Carlo
• From plane waves to local Gaussians for the simulation of correlated periodic systems
• Quartic scaling MP2 for solids: A highly parallelized algorithm in the plane wave basis
• Static and dynamical correlation in diradical molecules by Quantum Monte Carlo using the Jastrow Antisymmetrized Geminal Power ansatz
• Evidence for Stable Square Ice from Quantum Monte Carlo
• How strongly do hydrogen and water molecules stick to carbon nanomaterials?
• Benchmarking the performance of Density Functional Theory and Point Charge Force Fields in their Description of sI Methane Hydrate against Diffusion Monte Carlo
• Singles correlation energy contributions in solids
• A comparison between quantum chemistry and quantum Monte Carlo techniques for the adsorption of water on the (001) LiH surface
• Toward Accurate Adsorption Energetics on Clay Surfaces
• Molecular properties by Quantum Monte Carlo: an investigation on the role of the wave function ansatz and the basis set in the water molecule
• Systematic study of finite-size effects in quantum Monte Carlo calculations of real metallic systems
• Bulk and surface energetics of lithium hydride crystal: benchmarks from quantum Monte Carlo and quantum chemistry
• Systematically convergent method for accurate total energy calculations with localized atomic orbitals
• Water on BN doped benzene: A hard test for exchange-correlation functionals and the impact of exact exchange on weak binding
• Properties of Reactive Oxygen Species by Quantum Monte Carlo

Cited by in corpus (20)

• Interactions between Large Molecules: Puzzle for Reference Quantum-Mechanical Methods
• On the physisorption of water on graphene: Sub-chemical accuracy from many-body electronic structure methods
• Coupled cluster theory in materials science
• Applying the Coupled-Cluster Ansatz to Solids and Surfaces in the Thermodynamic Limit
• Interaction between water and carbon nanostructures: How good are current density functional approximations?
• A new scheme for fixed node diffusion quantum Monte Carlo with pseudopotentials: improving reproducibility and reducing the trial-wave-function bias
• Chemi-sorbed versus physi-sorbed surface charge and its impact on electrokinetic transport: carbon versus boron-nitride surface
• Hydration of NH${}_4^{+}$ in Water: Bifurcated Hydrogen Bonding Structures and Fast Rotational Dynamics
• Surface science using coupled cluster theory via local Wannier functions and in-RPA-embedding: the case of water on graphitic carbon nitride
• Efficient and accurate description of adsorption in zeolites
• Random Phase Approximation Applied to Many-Body Noncovalent Systems
• Systematic discrepancies between reference methods for non-covalent interactions within the S66 dataset
• New insights into the 1D carbon chain through the RPA
• Basis set incompleteness errors in fixed-node diffusion Monte Carlo calculations on non-covalent interactions
• Approaching the basis-set limit of the dRPA correlation energy with explicitly correlated and Projector Augmented-wave methods
• ByteQC: GPU-Accelerated Quantum Chemistry Package for Large-Scale Systems
• Understanding the wetting of transition metal dichalcogenides from an ab initio perspective
• Beyond single-reference fixed-node approximation in ab initio Diffusion Monte Carlo using antisymmetrized geminal power applied to systems with hundreds of electrons
• Assessing many-body methods on the potential energy surface of the (H${}_2$)${}_2$ hydrogen dimer
• Cooperative CO${}_2$ capture via oxalate formation on metal-decorated graphene