The details including the methods, techniques, instruments and chemical reagents used the experiments are detailed in the article published in American Chemical Society (ACS) Journal: Applied Energy Materials Article Title: Photovoltaic Performance of Phase-Pure Orthorhombic BiSI Thin-Films Authors: Devendra Tiwari, Fabiola Cardoso-Delgado, Dominic Alibhai, Maia Mombrú, and David J. Fermín DOI:10.1021/acsaem.9b00544 14 different files are provided with this key: - 13 of them are in .CSV format and can be viewed using any text editor or any spreadsheet software (1-11 & S1). - 1 of them is in .tiff picture format and viewed using any image visualization software (12). Different data acquired from different experimental techniques are categorized under tabs names listed as follows: 1. XRD: X-ray diffraction data for BiSI film on Glass substrate. 2. Measured_RamanSpectrum: Raman spectrum data for BiSI film measured in the range of 83 to 200 wavenumbers under 785 nm laser excitation. 3. Calculated_RamanSpectrum:Raman spectrum of BiSI calculated using density functional perturbation theory (DFPT) 4. transmittance_Reflectance: transmittance and reflectance spectrum data for BiSI film on Glass substrate measured in the wavelength range of 600 to 1100 nm. 5. Photoluminiscence_spectrum: data consisting the area normalized capacitance as function of potential (scaled vs. SHE) of BiSI film on fluorine doped tin oxide (FTO) coated Glass substrate for the Mott-Schottky plot 6. BandStructure: Bandstructure of BiSI calculated using quasiparticle GW approximation. 7. DensityOfStates: Density of states of BiSI calculated using quasiparticle GW approximation. 8. MottSchottkyPlot_BiSI: data consisting the area normalized capacitance as a function of potential (scaled vs. SHE) of BiSI film on fluorine doped tin oxide (FTO) coated Glass substrate for the Mott-Schottky plot. 9. Light_JV: data consisting the current-voltage characteristics of solar cell fabricated using BiSI from gas phase iodination with architecture: Glass/FTO/SnO2/BiSI/F8/Au under simulated AM 1.5G spectrum. 10. EQE: data consisting the light wavelength dependent response of the best solar cell fabricated using BiSI from gas phase iodination with architecture: Glass/FTO/SnO2/BiSI/F8/Au. 11. TimeResolvedPL: Time resolved Photoluminescence data for BiSI film on fluorine doped tin oxide (FTO) coated Glass substrate. 12. SEM_BiSI.tif: Scanning electron micrographa acquired on the Top surface of BiSI film at two different magnifications. This file can be accessed with most common image viewinng programs. S1. MottSchottkyPlot_SnOx: data consisting the area normalized capacitance as a function of potential (scaled vs. SHE) of SnOx film on fluorine doped tin oxide (FTO) coated Glass substrate for the Mott-Schottky plot.