This file contains the raw dataset used in the manuscript "Tailored Nanoscale Plasmon-Enhanced Vibrational Electron Spectroscopy" published in L. H. G. Tizei et al Nano Letters, 2020 (doi: 10.1021/acs.nanolett.9b04659) Data has been acquired using Nion Swift (https://nionswift.readthedocs.io/en/stable/). Experimental details can be found in L. H. G. Tizei et al Nano Letters, 2020 (doi: 10.1021/acs.nanolett.9b04659). The dataset has been analyzed using the following Python libraries: Numpy, Scipy, Hyperspy, Matplotlib EELS hyperspectral images have been aligned using the Hyperspy "align1D" method. Aligned EELS hyperspectral images are saved in files finished with "_Aligned.hspy": For the strong coupling experiments: Tip 1 is on hBN Tip 2 is on vacuum For each of the nanowires tips, a file with the fitted coefficients are available, as well as a plot of the data and the fitted curve. Datasets have been fitted with gaussian and/or lorentizan functions, as described in the published text. Any question can be forwarded to the corresponding authors of the published text.

Other funding: 1) National Agency for Researchunder the program of future investment TEMPOS-CHROMATEM (reference no. ANR-10-EQPX-50); 2) Spanish MINECO (MAT2017-88492-R and SEV2015-0522); 3) the Catalan CERCA Program; 4) Fundació Privada Celle;