Optimized spectroscopic scheme for enhanced precision CO measurements with applications to urban source attribution

Abstract:

Carbon monoxide (CO) is an urban pollutant generated by internal combustion engines which contributes to the formation of ground level ozone (smog). CO is also an excellent tracer for emissions from mobile combustion sources. In this work we present an optimized spectroscopic sampling scheme that enables enhanced precision CO measurements. The scheme was implemented on the Picarro G2401 Cavity Ring-Down Spectroscopy (CRDS) analyzer which measures CO₂, CO, CH₄ and H₂O at 0.2 Hz. The optimized scheme improved the raw precision of CO measurements by 40% from 5 ppb to 3 ppb. Correlations of measured CO₂, CO, CH₄ and H₂O from an urban tower were partitioned by wind direction and combined with a concentration footprint model for source attribution. The application of a concentration footprint for source attribution has several advantages. The upwind extent of the concentration footprint for a given sensor is much larger than the flux footprint. Measurements of mean concentration at the sensor location can be used to estimate source strength from a concentration footprint, while measurements of the vertical concentration flux are necessary to determine source strength from the flux footprint. Direct measurement of vertical concentration flux requires high frequency temporal sampling and increases the cost and complexity of the measurement system.