摘要： Time-gated picosecond laser-induced breakdown spectroscopy (ps-LIBS) for the determination of local equivalence ratios in atmospheric-pressure adiabatic methane–air flames is demonstrated. Traditional LIBS for equivalence-ratio measurements employ nanosecond (ns)-laser pulses, which generate excessive amounts of continuum, reducing measurement accuracy and precision. Shorter pulse durations reduce the continuum emission by limiting avalanche ionization. Furthermore, by contrast the use of femtosecond lasers, plasma emission via picosecond-laser excitation has high signal-to-noise ratio (S/N), allowing single-shot measurements suitable for equivalence-ratio determination in turbulent reacting flows. We carried out an analysis of the dependence of the plasma emission ratio Hα (656 nm)/NII (568 nm) on laser energy and time-delay for optimization of S/N and minimization of measurement uncertainties in the equivalence ratios. Our finding shows that higher laser energy and shorter time delay reduces measurement uncertainty while maintaining high S/N. In addition to atmospheric-pressure flame studies, we also examine the stability of the ps-LIBS signal in a high-pressure nitrogen cell. The results indicate that the plasma emission and spatial position could be stable, shot-to-shot, at elevated pressure (up to 40 bar) using a lower excitation energy. Our work shows the potential of using ps-duration pulses to improve LIBS-based equivalence-ratio measurements, both in atmospheric and high-pressure combustion environments.