The Importance of Capturing Local Measurement-Driven Adjustment of Modelled j(NO2)

ATMOSPHERE(2022)

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摘要
Accurate photolysis rate constants are essential for simulation of local air quality but their values can vary substantially with changes in local meteorological and surface conditions. This study demonstrates the use of local radiometer measurements for capturing via hourly measurement-driven adjustment factors (MDAF) the temporal resolution needed to adjust clear-sky or cloud-free model estimates of j(NO2). Measurements simultaneously at two sites in the UK (Auchencorth Moss and Manchester) showed that TUV (v5.3) model estimates of j(NO2)down arrow in cloud-free conditions (used as an example of modelled j-values) were, on average, approximately 45% larger than measured j(NO2)down arrow, which would lead to substantial model bias in the absence of local adjustment. At Auchencorth Moss, MDAF values based on 4 pi and 2 pi radiometer inlets generally agreed very well with each other (<6% average difference). However, under conditions of particularly high surface albedo (such as snow cover), increased upwelling local diffuse radiation yielded an MDAF derived using total radiation (sum of down arrow and up arrow components) similar to 40% larger than the MDAF derived using only down arrow radiation. The study has demonstrated: (1) the magnitude of potential impact of local conditions-principally cloud cover, but also changes in surface albedo-on assumed j-values; (2) that whilst annual mean MDAF values are similar at Auchencorth Moss and Manchester, there is no contemporaneous correlation between them at hourly resolution; hence MDAF values derived at one site cannot readily be applied at another site. These data illustrate the need to routinely deploy long-term radiometer measurements alongside compositional measurements to support atmospheric chemistry modelling.
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关键词
atmospheric photolysis, j-value, photolysis constant, surface albedo, TUV model
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