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Owing to climate change issues caused by global warming, the role of alternative fuels, such as low-carbon and non-carbon fuels, is becoming increasingly important, particularly in the transportation sector. Therefore, hydrogen has emerged as a promising fuel for internal combustion engines because it does not emit carbon dioxide. Direct injection is mandatory for hydrogen-based internal combustion engines to mitigate backfires and low energy density. However, there is a lack of measurement of the equivalence ratio methodology because hydrogen has a higher diffusion rate than conventional fuels. The objective of this research is a feasibility study of laser-induced breakdown spectroscopy (LIBs) for measuring the equivalence ratio. The second harmonic ND-YAG laser was implemented to induce the atomic emission of hydrogen via the breakdown phenomenon. Simultaneously, the hydrogen jet structure was visualized in a constant volume vessel using Schlieren imaging.