CuInS_2 (CIS) thin films were deposited on Mo-coated glass substrates using in situ sulfurization of thermally evaporated precursor Cu-In alloys. Samples were removed before, during and after the sulfurization for X-ray diffractometry (XRD) and Raman spectroscopy analysis. While various phases, including the desired CIS, can be identified by XRD, we show that only Raman spectroscopy can reveal the existence of the two structure orders of the CIS phase, namely the CuInS_2-chalcopyrite and the CuInS_2-CuAu metastable structure orders. Furthermore, this study also provides direct evidence to show that the CIS phase grows at the expense of an intermediate Cu_(11)In_9 phase.
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