W. Walters, Masayuki Takeuchi, N. L. Ng, Meredith G. Hastings
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引用次数: 0
Abstract
Abstract. The oxygen isotope anomaly (Δ17O = δ17O − 0.52 × δ18O > 0) has proven to be a robust tool for probing photochemical cycling and atmospheric formation pathways of oxidized reactive nitrogen (NOy). Several studies have developed modeling techniques to implicitly model Δ17O of NOy molecules based on numerous assumptions that may not always be valid. Thus, these models may be oversimplified and limit our ability to compare model Δ17O values of NOy with observations. In this work, we introduce a novel method for explicitly tracking Δ17O transfer and propagation into NOy and odd oxygen (Ox), integrated into the Regional Atmospheric Chemistry Mechanism, version 2 (RACM2). Termed ICOIN-RACM2 (InCorporating Oxygen Isotopes of NOy in RACM2), this new model includes the addition of 55 new species and 729 replicate reactions to represent the propagation of Δ17O derived from O3 into NOy and Ox. Employing this mechanism within a box model, we simulate Δ17O for various NOy and Ox molecules for chamber experiments with varying initial nitrogen oxides (NOx = NO + NO2) and α-pinene conditions, revealing response shifts in Δ17O linked to distinct oxidant conditions. Furthermore, diel cycles are simulated under two summertime scenarios, representative of an urban and rural site, revealing pronounced Δ17O diurnal patterns for several NOy components and substantial Δ17O differences associated with pollution levels (urban vs. rural). Overall, the proposed mechanism offers the potential to assess NOy oxidation chemistry in chamber studies and air quality campaigns through Δ17O model comparisons against observations. The integration of this mechanism into a 3-D atmospheric chemistry transport model is expected to notably enhance our capacity to model and anticipate Δ17O across landscapes, consequently refining model representations of atmospheric chemistry and tropospheric oxidation capacity.
期刊介绍:
Geoscientific Model Development (GMD) is an international scientific journal dedicated to the publication and public discussion of the description, development, and evaluation of numerical models of the Earth system and its components. The following manuscript types can be considered for peer-reviewed publication:
* geoscientific model descriptions, from statistical models to box models to GCMs;
* development and technical papers, describing developments such as new parameterizations or technical aspects of running models such as the reproducibility of results;
* new methods for assessment of models, including work on developing new metrics for assessing model performance and novel ways of comparing model results with observational data;
* papers describing new standard experiments for assessing model performance or novel ways of comparing model results with observational data;
* model experiment descriptions, including experimental details and project protocols;
* full evaluations of previously published models.