Research data supporting 'Transient Au-Cl adlayers modulate the surface chemistry of gold nanoparticles during redox reactions'

This dataset originates from a study investigating nanoscale surface chemistry at gold nanoparticle (AuNP) interfaces, with particular focus on the role of transient Au-Cl adlayers in stabilizing and regenerating sub-nanometre plasmonic gaps. The work aimed to understand how chloride ions, surface oxidation, and ligand rebinding processes govern the reproducibility and stability of surface-enhanced Raman scattering (SERS) substrates. Data were obtained using multi-layered AuNP aggregates ('MLagg') assembled with cucurbit[n]uril (CB[n]) linkers. Spectro-electrochemical experiments included time-resolved SERS (785 nm excitation), cyclic voltammetry, open-circuit potential (OCP) monitoring, X-ray photoelectron spectroscopy (XPS), dark-field scattering, and electron microscopy. Density functional theory (DFT) calculations were also performed to model the Au oxide lattice and Au-Cl bonding, vibrational modes, and charge redistribution. The dataset includes raw and processed SERS spectra, OCP and CV traces, XPS data, extracted vibrational peak assignments, and DFT input/output files. Metadata cover electrolyte composition, applied potentials, scan rates, and ligand concentrations. These data provide a reusable resource for understanding interfacial redox processes, ligand binding, and nanoparticle stabilization, with applications in sensing, catalysis, and colloidal growth.