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InGaPBi crystalline thin films with up to 2.1% bismuth concentration have been grown on GaAs substrates by molecular beam epitaxy. Rutherford backscattering spectrometry confirms that the majority of Bi atoms are located at substitutional lattice sites. The films exhibit good surface, structural, and interface quality, and their strains can be tuned from tensile to compressive by increasing the Bi content. InBi LO and GaBi LO vibrational modes in Raman spectroscopy were observed, and their intensities increased with Bi concentration. A weak photoluminescence signal was observed at 1.78 eV at room temperature for the sample with a Bi content of 0.5%.