This paper presents a measurement system based on the first harmonic in tunable diode laser absorption spectroscopy using a vertical-cavity surface-emitting laser to measure the atmospheric CO2 and H2O concentrations. The developed system separates the residual amplitude modulation signal from the harmonics and then eliminates it. A digital signal processing is developed to autonomously infer the wavelength and light intensities of the laser. The gas concentrations are determined without extra calibration. The long-term measurements are taken to validate the precision and accuracy of the system. Based on the Allan variance analysis, the broad wavelength scanning enhances the measurement precision, and the first-harmonic detection can achieve about two times as high precision as the traditional second-harmonic detection. The field measurements implemented in early spring of 2018 in Munich were compared with the commercial nondispersive infrared (NDIR) sensor. The outcomes have revealed that our system has high accuracy for the gas concentration measurements and high consistency with the NDIR sensor. The diurnal variations of CO2 concentration have demonstrated that CO2 concentration in urban areas is affected by the biosphere and meteorological conditions and the daily anthropogenic activities. Furthermore, the air trajectory analysis based on the HYSPLIT model has found that the CO2 emission sources primarily come from the southeast of Munich. The developed system described in this paper has a great potential for in situ trace gas concentration measurements, the analysis on the polluted gas distributions, and the verification of the pollutant transport model in urban areas.
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