The local environments of CAs acceptors in InxGa1−xAs and AlxGa1−xAs have been determined from the localized vibrational modes (LVMs) of both isolated CAs impurities and H-CAs pairs using infrared (IR) absorption and Raman scattering techniques. In as-grown layers of InxGa1−xAs (x<0.1), a single LVM due to isolated CAs acceptors was observed. The introduction of hydrogen led to the formation of H-CAs pairs and a single A1−-mode (stretch) and a single A1+-mode (XH) were observed for the InxGa1−xAs layers. All the LVMs were identified with carbon in CAsGa4 cluster configurations implying that less than 5 % of the detectable carbon atoms were present in clusters incorporating one or more CAs-In bonds. For AlxGa1−xAs, five stretch modes and five X-modes of the H-CAs pairs were observed for 0<x<1 and each mode was assigned to configurations for which the originally unpaired CAs had 0,1,2,3 or 4 Al nearest neighbors. These results show that carbon does not appear to form bonds with In atoms for the InxGa1−xAs samples investigated and this can explain the difficulty found in incorporating CAs acceptors in InxGa1−xAs with x>0.1 for some growth techniques. CAs acceptors can form strong bonds with both Al and Ga atoms, however, leading to a high solubility of carbon in AlxGa1-xAs over the full compositional range.