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signed in the literature to monoclinic VO2 (e.g., see Reference [201]), along with peaks belonging to the Si substrate (305 and 520 cmâ1 ). The peaks near 195 cmâ1 and 225 VO2 Film on Si @ 54 ºC  3 10x10 4 820 670 Si 620 440 5 390,395 6 Si 340 7 265 8 195 225 Intensity (arb. units) 9 200 300 400 500 600 700 800 -1 Raman shift (cm ) Figure 5.2: Representative Raman spectrum of the witness film in the monoclinic (lowtemperature) phase, showing several characteristic VO2 peaks and two Si-substrate peaks. cmâ1 correspond to characteristic Ag -symmetry vibrational modes of the monoclinic (lowtemperature) structure of VO2 , which vanish upon transition into the tetragonal (hightemperature) phase.195â197, 201 These phonon modes play a crucial role in the structural transition of VO2 , since they are associated with the pairing and tilting motions of VâV dimers that map the monoclinic onto the tetragonal lattice configuration. 31 In addition, the complete disappearance of the 195 cmâ1 peak at sufficiently high temperatures indicates that our VO2 material does not contain measurable amounts of the V2 O5 phase,198 the terminal oxidation state of vanadium, which has a distinctive Raman line at 196 cm â1 . 131