1. Summary
This repository contains key raw data from the computational-modelling component of the study reported in the manuscript:

M. J. Bryant, J. M. Skelton, L. E. Hatcher, C. Stubbs, E. Madrid, A. R. Pallipurath, L. H. Thomas, C. H. Woodall, J. Christensen, S. Fuertes, T. P. Robinson, C. M. Beavers, S. J. Teat, M. R. Warren, F. Pradaux-Caggiano, A. Walsh, F. Marken, D. R. Carbery, S. C. Parker, N. B. McKeown, R. Malpass-Evans, M. Carta and P. R. Raithby, “A rapidly-reversible absorptive and emissive vapochromic Pt(II) pincer-based chemical sensor”, Nature Communications 8, 1800 (2017), DOI: 10.1038/s41467-017-01941-2

	This manuscript and the associated supporting information are open access and available to view and download free of charge on the journal website.

2. Overview
The files in this repository provide raw data from the computational modelling presented in the above article. The set of data includes the optimised structures and calculated energy-level spectra and dielectric properties of the three solid-state forms of compound 1 (Form-I/hydrated, Form-II/anhydrous and Form-III/methanolic), together with the optimised structures of the gas-phase molecular models used to calculate complexation and formation energies.
For brevity, we have only included the data discussed in the main text, and we have omitted data from calculations carried out with the PBEsol + D3 (BJ) and PBE0 + D3 (BJ) functionals. This data, and any other data not included in this repository or attached to the article as supporting information, may be obtained from the authors on request. We can also supply input files for the calculations on request.

3. Available Data
	The data is organised into four subfolders, one each for Form-I, Form-II and Form-III, and one for the molecular models used to calculate formation and complexation energies. For ease of downloading, the folders have been packed into GZip-compressed TAR format archives named Form-{I, II, III}.tar.gz and MolecularModels.tar.gz These can be unpacked using the tar utility on macOS and Linux, or the free PeaZip software on Windows (http://www.peazip.org/, accessed 25/01/2018). Each archive contains the following files:

3.1 Optimised structures: *.vasp
These files contain the optimised structures of the three solid-state forms of 1 in the Vienna ab initio Simulation Package (VASP) POSCAR format, together with the 113 supercell expansions used to visualise the highest-occupied and lowest-unoccupied crystal orbitals (HOCOs/LUCOs) and to generate the images in Figure 4d in the text and Supplementary Figure S16 in the supporting information.
In the molecular models archive, the optimised structures of the gas-phase models of the Pt-“pincer” complex, H2O, MeOH, and the dimeric molecular complexes in the Form-I, Form-II and Form-III crystal structures are given. These were used to calculate the formation and complexation energies quoted in the text and presented in Supplementary Tables S2 and S3 in the supporting information.
Further information about the POSCAR format may be found in the VASP documentation at https://www.vasp.at/ (accessed 25/01/2018).

3.2 Orbital energy levels: Form-{I, II, III}_EnergyLevels.csv
	These files contain the calculated core-level eigenvalues and electronic band energies of the three solid-state forms of compound 1. This information was used to generate the energy-level spectra shown in Supplementary Figure S17 in the supporting information. 

3.3 Dielectric properties: Form-{I, II, III}_*.csv
	These files contain the calculated frequency-dependent imaginary and real dielectric functions of the three solid-state forms of 1 (, ) and three derived quantities, viz. the refractive index , the extinction coefficient  and the absorption coefficient .
	The frequency-dependent real and imaginary dielectric tensors obtained directly from the calculations are stored in files suffixed with DielectricTensors. A second set of files suffixed with DielectricData contain ,  and the derived properties calculated along the three Cartesian directions (, , ), while a third set suffixed with AverageDielectricData contain isotropic averages calculated as .
	The isotropically-averaged absorption coefficients as a function of wavelength from the latter set of files are displayed in Supplementary Figure 18 in the supporting information.
	All three files are in the plain-text comma-separated values (CSV) format, and can be viewed in a text editor or visualised using a suitable spreadsheet/visualisation package.