Abstract

Abstract. Carbon monoxide (CO) is an important pollutant in urban agglomerations. Quantifying the total burden of this pollutant in a megacity is challenging because not only its surface concentration but also its vertical dispersion present different behaviours and high variability. The diurnal trend of columnar CO in the boundary layer of Mexico City has been measured during various days with ground-based infrared absorption spectroscopy. Daytime CO total columns are retrieved from solar spectra and for the first time, nocturnal CO total columns using moonlight have been retrieved within a megacity. The measurements were taken at the Universidad Nacional Autónoma de México (UNAM) campus located in Mexico City (19.33° N, 99.18° W, 2260 m a.s.l.) from October 2007 until February 2008 with a Fourier-transform infrared spectrometer at 0.5 cm−1 resolution. The atmospheric CO background column was measured from the high altitude site Altzomoni (19.12° N, 98.65° W, 4010 m a.s.l.) located 60 km southeast of Mexico City. The total CO column within the city presents large variations. Fresh CO emissions at the surface, the transport of cleaner or more polluted air masses within the field-of-view of the instrument and other processes contribute to this variability. The mean background value above the boundary mixing layer was found to be (8.4±0.5)×1017 molecules/cm2, while inside the city, the late morning mean on weekdays and Sundays was found to be (2.73±0.41)×1018 molecules/cm2 and (2.04±0.57)×1018 molecules/cm2, respectively. Continuous CO column retrieval during the day and night (when available), in conjunction with surface CO measurements, allow for a reconstruction of the effective mixing layer height. The limitations from this simplified approach, as well as the potential of using continuous column measurements in order to derive top-down CO emissions from a large urban area, are discussed. Also, further monitoring will provide more insight in daily and weekly emission patterns and a usable database for the quantitative validation of CO from satellite observations in a megacity.

Highlights

  • Ambient concentrations of carbon monoxide (CO) are variable and have changed significantly since industrialization

  • This paper presents the retrieved total column of urban carbon monoxide measured during daytime from solar infrared spectra and for the first time, the CO column in a megacity has been measured during the night from a ground-based instrument

  • The CO column was measured in Mexico City between October 2007 and February 2008 and the results are presented

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Summary

Introduction

Ambient concentrations of carbon monoxide (CO) are variable and have changed significantly since industrialization. This paper presents the retrieved total column of urban carbon monoxide measured during daytime from solar infrared spectra and for the first time, the CO column in a megacity has been measured during the night from a ground-based instrument Both types of measurements, when the conditions are satisfied, provide a continuous time series of the column which provides new insight into the nocturnal structure of the atmosphere. Using this information, diurnal patterns of the CO budget are investigated during different periods, the height and evolution of the mixing layer can be monitored under specific conditions and a new approach for estimating the effective emission of CO in Mexico City is proposed

Measurement realization
Instrumentation
Solar measurements
Lunar measurements
CO column retrieval
Retrieval diagnostics and error estimation
Smoothing error
Temperature error
Error in the ILS
Random errors
Experimental evaluation of the retrieved CO column
Results
Total CO column measurements above the boundary layer
Day to day variations of the CO columns within Mexico City
Diurnal and nocturnal behaviour of the CO column
MLH estimation
MLH reconstruction
Error and sensitivity of the retrieved MLH
Mixing layer height comparison
Impact of the CO residual layer on the MLH reconstruction
Conclusions
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