Abstract. Detailed knowledge about the urban NO2 concentration field
is a key element for obtaining accurate pollution
maps and individual exposure estimates. These are required for improving the understanding of the impact of ambient
NO2 on human health and for related air quality measures. However, city-scale NO2 concentration maps
with high spatio-temporal resolution are still lacking, mainly due to the difficulty of accurate measurement of
NO2 at the required sub-ppb level precision. We contribute to close this gap through the development of
a compact instrument based on mid-infrared laser absorption spectroscopy. Leveraging recent advances in infrared laser
and detection technology and a novel circular absorption cell, we demonstrate the feasibility and robustness of this
technique for demanding mobile applications. A fully autonomous quantum cascade laser absorption spectrometer (QCLAS) has
been successfully deployed on a tram, performing long-term and real-time concentration measurements of NO2 in
the city of Zurich (Switzerland). For ambient NO2 concentrations, the instrument demonstrated a precision of
0.23 ppb at one second time resolution and of 0.03 ppb after 200 s averaging. Whilst the combined
uncertainty estimated for the retrieved spectroscopic values was less than 5 %, laboratory intercomparison
measurements with standard CLD instruments revealed a systematic NO2 wall loss of about 10 % within the
laser spectrometer. For the field campaign, the QCLAS has been referenced to a CLD using urban atmospheric air, despite
the potential cross sensitivity of CLD to other nitrogen containing compounds. However, this approach allowed a direct
comparison and continuous validation of the spectroscopic data to measurements at regulatory air quality monitoring (AQM)
stations along the tram-line. The analysis of the recorded high-resolution time series allowed us to gain more detailed
insights into the spatio-temporal concentration distribution of NO2 in an urban environment. Furthermore, our
results demonstrate that for reliable city-scale concentration maps a larger data set and better spatial coverage is
needed, e.g., by deploying more mobile and stationary instruments to account for mainly two shortcomings of the current
approach: (i) limited residence time close to sources with large short-term NO2 variations, and
(ii) insufficient representativeness of the tram tracks for the complex urban environment.