We report in this paper the development of an embedded ultralight spectrometer (<3 kg) based on tuneable diode laser absorption spectroscopy (with a sampling rate of 24 Hz) in the mid-infrared spectral region. This instrument is dedicated to in situ measurements of the vertical profile concentrations of three main greenhouse gases – carbon dioxide (CO2), methane (CH4) and water vapour (H2O) – via standard weather and tethered balloons. The plug and play instrument is compact, robust, cost-effective, and autonomous. The instrument also has low power consumption and is non-intrusive. It was first calibrated during an in situ experiment on an ICOS (Integrated Carbon Observation System) site for several days, then used in two experiments with several balloon flights of up to 30 km altitude in the Reims region of France in 2017–2018 in collaboration with Météo-France CNRM (Centre National de Recherches Météorologiques). This paper shows the valuable interest of the data measured by the AMULSE (Atmospheric Measurements by Ultra-Light Spectrometer) instrument during the APOGEE (Atmospheric Profiles of Greenhouse Gases) measurement experiment, specifically for the vertical profiles of CO2 and CH4, measurements of which remain very sparse. We have carried out several experiments showing that the measured profiles have several applications: the validation of simulations of infrared satellite observations, evaluating the quality of chemical profiles from chemistry transport models (CTMs) and evaluating the quality of retrieved chemical profiles from the assimilation of infrared satellite observations. The results show that the simulations of infrared satellite observations from IASI (Infrared Atmospheric Sounding Interferometer) and CrIS (Cross-track Infrared Sounder) instruments performed in operational mode for numerical weather prediction (NWP) by the radiative transfer model (RTM) RTTOV (Radiative Transfer for the TIROS Operational Vertical Sounder) are of good quality. We also show that the MOCAGE (Modèle de Chimie Atmosphérique de Grande Echelle) and CAMS (Copernicus Atmospheric Monitoring Service) CTMs modelled ozone profiles fairly accurately and that the CAMS CTM represents the methane in the troposphere well compared to MOCAGE. Finally, the measured in situ ozone profiles allowed us to show the good quality of the retrieved ozone profiles by assimilating ozone-sensitive infrared spectral radiances from the IASI and CrIS.