Today, ground-based optical remote sensing (ORS) has become an intensively used method for quantifying pollutant or greenhouse gas emissions from point or area sources, and for the validation of airborne or satellite remote sensing data. In this study, we present the results of a release experiment using acetylene (C2H2) as a tracer gas, where three ORS techniques were simultaneously tested for two main purposes: (1) the detection of emission sources and (2) the quantification of release rates. Therefore, passive and active open-path Fourier transform infrared spectroscopy (OP-FTIR) and open-path tunable diode laser absorption spectroscopy (TDLAS) were applied and evaluated. The concentration results of the active ORS methods are compared to those estimated by a Lagrangian stochastic atmospheric dispersion model. Our results reveal that passive OP-FTIR is a valuable tool for the rapid detection and imaging of emission sources and the spatial tracer gas distribution; while with active OP-FTIR and TDLAS, C2H2 concentrations in the sub-ppm range could be quantified that correlated well with the concentration data obtained by our modeling approach.