Data in association with the article "Collective Microscopic Dynamics in Aqueous LiTFSI from Dilute to Water-in-Salt Electrolytes: Insights from Quadrupolar NMR Relaxation and Molecular Simulations"

# Data Repository for the publication: Collective Microscopic Dynamics in Aqueous LiTFSI from Dilute to Water-in-Salt Electrolytes: Insights from Quadrupolar NMR Relaxation and Molecular Simulations (J. Phys. Chem. B, 2026) Article DOI: https://doi.org/10.1021/acs.jpcb.6c04931 This repository contains sample input files for the MD simulations, the generated MD trajectories, and data used to generate the figures in the main article. ## Folder Structure The folder `mw_input_files` contains the input files, for different molalities, used for the classical MD simulations with MetalWalls. The folder `fig` contains the data associated with the figures in the main article. Below is a description of the contents of each subfolder. ### figure2Contains the systems coordinates displayed in Figure 2 of the main text in LAMMPS trajectory format. ### figure3Contains subfolders for each panel (a-d), where each subfolder contains CSV files with the relevant quantities plotted in the corresponding panel. For panel 3b, sample files for a Müller-Plathe reverse non-equilibrium MD simulation are given in `example_rnemd`. For panel 3c-d, the diffusion coefficients are extracted from the position MSDs computed over 50 ns of classical MD trajectory. Here, the MSDs computed on a section of the full trajectory, as given in `figure5`, are provided, together with the final diffusion coefficients plotted in panels c-d. ### figure4Contains the trajectories used to compute the Li-O coordination numbers, together with a CSV file with the computed Li-O coordination numbers at different concentrations. ### figure5Contains the trajectories used to compute the Li-Li coordination numbers, together with a CSV file with the computed Li-Li coordination numbers at different concentrations. ### figure6Contains the occupancy matrices and survival functions for Li with water or with TFSI at different concentrations. The trajectories used to compute the residence times are the same as those provided for figure 5. ### figure7The DFT EFG at the Li site (`efg_li_{molality}m.npy`) and the classical EFG at the Li site (`efg_ext_li_{molality}m.npy`) are provided at different concentrations. The folders `example_qe` and `example_mw` contain examples (input and outputs) for a DFT QuantumESPRESSO calculation, and classical MetalWalls calculation, used to compute the EFG provided in the NPY files. The trajectories containing the frames on which the EFG was computed is also provided. ### figure8The files `efg_combined_{molality}m.npy` contain the classical EFGs while the time autocorrelation functions are stored in `acf_combined_{molality}m.npy`. The results presented in the article consider EFGs computed over 50 ns of classical MD simulations. A section of these is provided in the `figure5` folder. ### figure9Contains a CSV file providing the fast, slow, and tail contributions to $\tau_c$ at different concentrations, computed on the EFGs given in `figure8`. ### figure10 Contains a CSV file providing the experimental and simulation relaxation rates at different concentrations. ### figure11Contains a CSV file containing the viscosity, relaxation rates, and viscosity-normalized relaxation rates at different concentrations. ### figure12Contains a CSV file with the EFG variance and $\tau_c$ values across the investigated molalities. ### figure13For figure 13a, the diffusion coefficients of Li are given in folder `figure 3`. The different tau plotted in figure13d are given in `figure13d.csv`. The stress time autocorrelation functions (ACFs) used to compute $\tau_{struct}$, reported in figure 13e, are given as `pressure_acf_{molality}m.npz`. The results presented in the article consider stress tensors computed over 50 ns of classical MD. The stress tensor and corresponding stress ACFs computed on a section of these (corresponding to trejectories provided in the `figure5` folder) are given. Finally, values for tau_struc in figure 13e are given in `tau_struct_vs_tau_c.csv`.