We use Raman spectroscopy to investigate the chemical species at a NiFe surface isolated from Si after oxygen evolution reaction with/without light irradiation with a standard AM 1.5G, 1-sun light source (Fig. ). The sample comprises a 10 nm NiFe alloy film deposited on silica glass without further treatment. We maintain the same deposition conditions of the NiFe alloy to ensure consistency. Raman spectroscopy in Fig. shows four broad peaks in the NiFe layer. The Raman shifts at 482.6 cm -1 and 556.1 cm -1 originate from the e g bending and A 1g stretching vibrations of Ni-O in disordered Ni(OH) 2 47, 48 ; while Raman shifts at 322.9 cm -1 and 682.1 cm -1 stem from the presence of disordered FeOOH/NiOOH species at the surface . The intensity of Raman peaks corresponding to Ni/FeOOH species relative to all the Ni/Fe species peaks shows a minor rise after 10 h CA testing compared with the as-fabricated NiFe nano-film. Conversely, when light irradiates the sample, we observe a significant increase in Ni/FeOOH peak intensity, demonstrating a strongly light-accelerated reconfiguration of NiFe oxyhydroxides in the NiFe alloy surface.