This dataset contains experimental data collected on chrysene, C18H12, in a diamond anvil cell at pressures up to 10 GPa and a temperature range of 30-300 C Experimental data: synchrotron source FTIR data collected at Beamline X01DC in 2009, using the instrumentation documented in "Stability of Coronene at High Temperature and Pressure," JOURNAL OF PHYSICAL CHEMISTRY B, Vol: 114, Pages: 15753-15758, ISSN: 1520-6106, doi: 10.1021/jp105020f. FTIR-microspectrometry in transmission was performed using synchrotron light at the Swiss Light Source operated in top-up mode. Thus the infrared intensity remains constant with time. The IR focus available at the end of the beamline was coupled to the side port of a Bruker Vertex 70 FTIR spectrometer with an f1 = 34 mm/f2 = 213 mm ellipsoidal mirror. The spectrometer, equipped with a KBr beamsplitter, was coupled to the input of a Bruker Hyperion IR microscope without any additional optics. The microscope was equipped with two ×15 gold-coated Cassegrain objectives. The illuminated region of the sample was determined by an aperture of some 20−45 μm × 20−45 μm. In order to reduce the effect of scattered light and to enhance contrast fidelity, an identical conjugate aperture was placed between the collecting optics and the nitrogen-cooled mercury−cadmium−telluride (MCT) detector. Resolution and number of coadded scans were 4 cm−1 and 256, respectively. Crystals were observed in parallel by use of white light and a charge-coupled device (CCD) camera. Each zip file contains data files in raw (OPUS) and plain text (.dpt) formats, and a pdf scane of the labbook, which provides a key to relate the file names to the pressure/temeprature of the sample. Raw files are provided for both the background and the sample; plain text files were created from processed files.