Summertime weekly cycles of observed and modeled NO _x and O _3 concentrations as a function of satellite-derived ozone production sensitivity and land use types over the Continental United States

摘要

To show how remote-sensing products can be used to classify the entire CONUS domain into "geographical regions" and "chemical regimes", we analyzed the results of simulation from the Community Multiscale Air Quality (CMAQ) model version 4.7.1 over the Conterminous United States (CONUS) for August 2009. In addition, we observe how these classifications capture the weekly cycles of ground-level nitrogen oxide (NO _x) and ozone(O3) at US EPA Air Quality System (AQS) sites. We use the Advanced Very High Resolution Radiometer (AVHRR) land use dominant categories and the Global Ozone Monitoring Experiment-2 (GOME-2) HCHO/NO _2 column density ratios to allocate geographical regions (i.e., "urban","forest", and "other" regions) and chemical regimes (i.e.,"NO _x-saturated", "NO _x-sensitive", and "mixed" regimes).We also show that CMAQ simulations using GOME-2 satellite-adjusted NO _x emissions mitigate the discrepancy between the weekly cycles of NO _x from AQS observations and that from CMAQ simulation results. We found geographical regions and chemical regimes do not show a one-to-one correspondence: the averaged HCHO/NO _2 ratios for AVHRR "urban" and "forest" regions are 2.1 and 4.0, which correspond to GOME-2 "mixed" and "NO _xsensitive"regimes, respectively. Both AQS-observed and CMAQ-simulated weekly cycles of NO _x show high concentrations on weekdays and low concentrations on weekends,but with one-or two-day shifts of weekly high peaks in the simulated results, which eventually introduces the shifts in simulated weekly-low O _3 concentration. In addition,whereas the high weekend O _3 anomaly is clearly observable at sites over the GOME-2 NO _x-saturated regime in both AQS and CMAQ, the weekend effect is not captured at sites over the AVHRR urban region because of the chemical characteristics of the urban sites (GOME-2 mixed regime). In addition, the weekend effect from AQS is more clearly discernible at sites above the GOME-2 NO _x-saturated regime than at other sites above the CMAQ NO _x-saturated regime, suggesting that the GOME-2-based chemical regime classification is more accurate than CMAQ-based chemical classification. Furthermore, the CMAQ simulations using the GOME-2-derived NO _x emissions adjustment (decreasing from 462 GgN to 426 GgN over the US for August 2009) show large reductions of simulated NO _x concentrations (particularly over the urban, or NO _x-saturated, regime), and mitigates the large discrepancies between the absolute amount and the weekly pattern of NO _x concentrations of the EPA AQS and those of the baseline CMAQ.