The following experimental data taken in the NanoPhotonics Group at the Cavendish Laboratory (University of Cambridge), collected between 01/10/2015 to 01/04/2016 Figure1 - Stokes time series Figure2 - anti-Stokes Stokes spectrum Figure2 - anti-Stokes Stokes time series Figure2 - DFT calculations - experimental spectra Figure3 - aS S power series Figure3 - aS power series Figure3 - phonon population Figure3 - coupling strengths Figure4 - laser switching Figure4 - laser power increase The following simulation data obtained at CSIC - UPV/EHU and DIPC between 01/04/2016 and 10/07/2016: Figure1 - Near-Field distribution Figure2 - DFT calculations - simulated spectra All datasets are in the .txt format and can be read using any data visualisation software (e.g. Micorsoft Excel, MatLab,...) Dataset for journal article "Single-molecule optomechanics in ‘pico-cavities’". Principal investigator: Jeremy J. Baumberg (jjb12@cam.ac.uk)