A Zeppelin airship was used as a platform for in situ measurements of greenhouse gases and short-lived air pollutants within the planetary boundary layer (PBL) in Germany. A novel quantum cascade laser-based multi-compound gas analyzer (MIRO Analytical AG) was deployed to simultaneously measure in situ concentrations of greenhouse gases (CO.sub.2, N.sub.2 O, H.sub.2 O, and CH.sub.4) and air pollutants (CO, NO, NO.sub.2, O.sub.3, SO.sub.2, and NH.sub.3) with high precision at a measurement rate of 1 Hz. These measurements were complemented by electrochemical sensors for NO, NO.sub.2, O.sub.x (NO.sub.2 + O.sub.3 ), and CO, an optical particle counter, temperature, humidity, altitude, and position monitoring. Instruments were operated remotely without the need for on-site interactions. Three 2-week campaigns were conducted in 2020 comprising commercial passenger as well as targeted flights over multiple German cities including Cologne, Mönchengladbach, Düsseldorf, Aachen, Frankfurt, but also over industrial areas and highways.