File Name : figure s1.tif Caption : figure s1. schematic diagram of the set-up used for cvd growth of 2d cr2s3 nanoflakes. File Name : figure s2 _a_.tif Caption : figure s2. (a) optical microscope image of cvd-grown 2d cr2s3 on mica substrate, where four different flakes are numbered. File Name : figure s2 _b_.tif Caption : figure s2. (b) afm images of those four numbered flakes together with their respective height profiles; File Name : figure s4.tif Caption : figure s4. deconvolution of two closely placed modes, p1 and p2, at temperatures 300k and 5k. File Name : figure s5.tif Caption : figure s5. schematic diagram of the experimental setup for, (a) linearly polarized raman spectroscopy; (b) circularly polarized raman spectroscopy. File Name : figure s6.tif Caption : figure s6. (a) linearly polarized raman spectroscopy for parallel (‖) and perpendicular (⏊) configurations measured at 5k and 300k; (b) schematic diagram of the experimental setup for angle resolved polarized raman spectroscopy.