Dataset of Noncovalent Interactions at Solid Electrolyte Interfaces Based on First-Principles and NCI-RDG Analysis

This dataset, derived from research on the microscopic formation mechanisms of the solid electrolyte interphase (SEI), systematically comprises adsorption configurations and electronic structure information for 18 typical electrolyte solvent and additive molecules (including cyclic carbonates, linear carbonates, sultones, and fluorinated additives) on four representative inorganic SEI crystal planes: Li₂CO₃(001), Li₂O(111), LiF(001), and LiOH(001).The initial molecular and crystal structure models were primarily constructed using Materials Studio, with a 20 Å vacuum layer added to the exposed inorganic surfaces to effectively eliminate periodic image interactions.All underlying physical computations were performed using density functional theory (DFT) via the Vienna Ab initio Simulation Package (VASP).Calculations were based on the projector augmented-wave (PAW) method and the PBE exchange-correlation functional within the generalized gradient approximation (GGA), incorporating DFT-D3 dispersion corrections to accurately describe weak interactions such as interfacial van der Waals forces.The plane-wave cutoff energy was set to 520 eV across all systems, with energy and force convergence criteria for structural optimization strictly maintained at 1×10⁻⁶ eV and 0.01 eV/Å, respectively.At the spatial scale, this dataset consists of atomic-level static thermodynamic simulations (with angstrom-level resolution) designed to reflect thermodynamically stable configurations during the initial stages of reaction; thus, it excludes macroscopic temporal or geospatial dynamic information.Regarding data processing and feature extraction, the Critic2 software was employed to conduct in-depth analysis of non-covalent interactions (NCI) and the reduced density gradient (RDG, defined as variable s) based on the electron density (∆ρ) output from VASP.By calculating the product of the sign of the second-largest eigenvalue of the Hessian matrix and the electron density (sign(λ₂)ρ), hydrogen bonding, strong dipole-dipole interactions, van der Waals forces, and steric effects within the systems were quantitatively and visually distinguished.Furthermore, the net interfacial charge transfer (∆Q) was extracted using the Bader topological charge partitioning method, complemented by calculations of the 3D differential charge density (∆ρ(r)) and the planar average differential charge density along the z-axis (∆ρ(z)).Tabular data within the dataset summarizes Bader charge transfer records for eight representative adsorption systems, where row labels denote specific solid-liquid interfaces (e.g., DEC-LiF, ES-Li₂O) and column labels record net charge transfer parameters in elementary charge units e (positive values indicate electron loss, negative values indicate electron gain).As these data originate from rigorous solutions of quantum mechanical equations with complete physical logical closure, the data missingness common in natural observational experiments is absent.Computational errors primarily stem from the theoretical limitations of the DFT method itself (such as the intrinsic bias of GGA functionals) and the theoretical approximation of simplifying complex room-temperature liquid electrolyte environments into isolated molecule-pure phase interfaces at absolute zero.The file structure of the dataset mainly covers the following categories: 3D atomic coordinate files (e.g., VASP POSCAR/CONTCAR formats recording structural parameters before and after relaxation), electronic structure files (CHGCAR format), and volumetric grid data files (.cub format) generated from NCI-RDG analysis.For the specialized data formats in computational chemistry, it is recommended to use Visual Molecular Dynamics (VMD) software for the visual rendering and image exportation of structural models, differential charge density isosurfaces (recommended value: 0.009 e/Å), and 3D RDG isosurfaces.The primary tool used for electron density topological analysis and RDG data processing is the open-source software Critic2.