Abstract. The offline Eulerian AURAMS (A Unified Regional Air quality Modelling System) chemical transport model was adapted to simulate airborne concentrations of seven PAHs (polycyclic aromatic hydrocarbons): phenanthrene, anthracene, fluoranthene, pyrene, benz[a]anthracene, chrysene + triphenylene, and benzo[a]pyrene. The model was then run for the year 2002 with hourly output on a grid covering southern Canada and the continental USA with 42 km horizontal grid spacing. Model predictions were compared to ~5000 24 h-average PAH measurements from 45 sites, most of which were located in urban or industrial areas. Eight of the measurement sites also provided data on particle/gas partitioning which had been modelled using two alternative schemes. This is the first known regional modelling study for PAHs over a North American domain and the first modelling study at any scale to compare alternative particle/gas partitioning schemes against paired field measurements. The goal of the study was to provide output concentration maps of use to assessing human inhalation exposure to PAHs in ambient air. Annual average modelled total (gas + particle) concentrations were statistically indistinguishable from measured values for fluoranthene, pyrene and benz[a]anthracene whereas the model underestimated concentrations of phenanthrene, anthracene and chrysene + triphenylene. Significance for benzo[a]pyrene performance was close to the statistical threshold and depended on the particle/gas partitioning scheme employed. On a day-to-day basis, the model simulated total PAH concentrations to the correct order of magnitude the majority of the time. The model showed seasonal differences in prediction quality for volatile species which suggests that a missing emission source such as air–surface exchange should be included in future versions. Model performance differed substantially between measurement locations and the limited available evidence suggests that the model's spatial resolution was too coarse to capture the distribution of concentrations in densely populated areas. A more detailed analysis of the factors influencing modelled particle/gas partitioning is warranted based on the findings in this study.
Hydrologic models have been used for numerous applications in the last number of decades. These applications include streamflow prediction, flood forecasting, or reservoir level forecasting, or in a scientific capacity to advance our understanding of hydrologic systems. Whether used in a predictive or scientific capacity, models are an abstraction of the complex natural system being simulated, and necessarily simplify the treatment of hydrological processes occurring in a watershed, either to facilitate computational expediency or in recognition of the large degree of uncertainty regarding how the watershed functions. In most practical cases, model calibration is required in order to reconcile model output with historical observation; conventionally, this calibration process focuses on tuning only model parameters. However, hydrologic models are typically considered to have four main components that contribute to model uncertainty (e.g., Beven, 2005;Butts et al., 2004;Gupta, Clark, et al., 2012): (1) input forcing data, such as precipitation and temperature, (2) model structure, which includes the algorithmic functions used to simulate the hydrologic cycle, (3) model parameters related to the selected hydrologic process algorithms (often the only degree of freedom used to tune model performance), and (4) an error term, which represents any uncertainty or deviation from reality not captured in the other three components of model uncertainty.This study focuses upon the simultaneous calibration of model structure and model parameters. We refer to model structure here as a combination of (a) the number and type of stores represented in the model and (b) the collection of algorithms used to describe the relationships between fluxes and storage in each hydrological response unit (HRU). Model structure can be further extended to other modeling decisions such as spatial discretization, but this extended definition is not evaluated here. Historically, most hydrologic models have been designed with a fixed model structure while the input data and model parameters may vary from watershed to watershed. These fixed model structures were typically chosen because they (1) adequately represented the hydrologic response of one or more watersheds, (2) generally respected the physics of water flow and storage, (3) were consistent with conceptual models of the water cycle garnered from field investigation, and/or (4) convention (Addor & Melsen, 2019). In many cases, trial and error was used to determine final model structure (e.g., Perrin et al., 2003). However, there are many such model structures that can generally meet these criteria, and as such, there exist dozens of fixed structure models which used different algorithms to represent various components of the water cycle. The fixed model structure concept
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