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Modelling chemistry in the nocturnal boundary layer above tropical rainforest and a generalised effective nocturnal ozone deposition velocity for sub-ppbv NOx conditions

Pugh, Thomas A.M. LU ; Ryder, James ; MacKenzie, A. Robert ; Moller, Sarah J. ; Lee, James D. ; Helfter, Carole ; Nemitz, Eiko ; Lowe, Douglas and Hewitt, C. Nicholas (2010) In Journal of Atmospheric Chemistry 65(2-3). p.89-110
Abstract

Measurements of atmospheric composition have been made over a remote rainforest landscape. A box model has previously been demonstrated to model the observed daytime chemistry well. However the box model is unable to explain the nocturnal measurements of relatively high [NO] and [O3], but relatively low observed [NO2]. It is shown that a one-dimensional (1-D) column model with simple O3-NOx chemistry and a simple representation of vertical transport is able to explain the observed nocturnal concentrations and predict the likely vertical profiles of these species in the nocturnal boundary layer (NBL). Concentrations of tracers carried over from the end of the night can affect the atmospheric... (More)

Measurements of atmospheric composition have been made over a remote rainforest landscape. A box model has previously been demonstrated to model the observed daytime chemistry well. However the box model is unable to explain the nocturnal measurements of relatively high [NO] and [O3], but relatively low observed [NO2]. It is shown that a one-dimensional (1-D) column model with simple O3-NOx chemistry and a simple representation of vertical transport is able to explain the observed nocturnal concentrations and predict the likely vertical profiles of these species in the nocturnal boundary layer (NBL). Concentrations of tracers carried over from the end of the night can affect the atmospheric chemistry of the following day. To ascertain the anomaly introduced by using the box model to represent the NBL, vertically-averaged NBL concentrations at the end of the night are compared between the 1-D model and the box model. It is found that, under low to medium [NOx] conditions (NOx<1 ppbv), a simple parametrisation can be used to modify the box model deposition velocity of ozone, in order to achieve good agreement between the box and 1-D models for these end-of-night concentrations of NOx and O3. This parametrisation would could also be used in global climate-chemistry models with limited vertical resolution near the surface. Box-model results for the following day differ substantially if this effective nocturnal deposition velocity for ozone is implemented; for instance, there is a 9% increase in the following days peak ozone concentration. However under medium to high [NO x] conditions (NOx > 1 ppbv), the effect on the chemistry due to the vertical distribution of the species means no box model can adequately represent chemistry in the NBL without modifying reaction rate coefficients.

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author
; ; ; ; ; ; ; and
publishing date
type
Contribution to journal
publication status
published
subject
keywords
Box model, NO, Nocturnal boundary-layer, Ozone, Rainforest
in
Journal of Atmospheric Chemistry
volume
65
issue
2-3
pages
22 pages
publisher
Springer
external identifiers
  • scopus:79959710295
ISSN
0167-7764
DOI
10.1007/s10874-011-9183-4
language
English
LU publication?
no
id
b8e0e9b5-c38f-4186-a5dd-5aca3e203911
date added to LUP
2020-11-19 23:31:34
date last changed
2022-02-01 17:58:47
@article{b8e0e9b5-c38f-4186-a5dd-5aca3e203911,
  abstract     = {{<p>Measurements of atmospheric composition have been made over a remote rainforest landscape. A box model has previously been demonstrated to model the observed daytime chemistry well. However the box model is unable to explain the nocturnal measurements of relatively high [NO] and [O<sub>3</sub>], but relatively low observed [NO<sub>2</sub>]. It is shown that a one-dimensional (1-D) column model with simple O<sub>3</sub>-NO<sub>x</sub> chemistry and a simple representation of vertical transport is able to explain the observed nocturnal concentrations and predict the likely vertical profiles of these species in the nocturnal boundary layer (NBL). Concentrations of tracers carried over from the end of the night can affect the atmospheric chemistry of the following day. To ascertain the anomaly introduced by using the box model to represent the NBL, vertically-averaged NBL concentrations at the end of the night are compared between the 1-D model and the box model. It is found that, under low to medium [NO<sub>x</sub>] conditions (NO<sub>x</sub>&lt;1 ppbv), a simple parametrisation can be used to modify the box model deposition velocity of ozone, in order to achieve good agreement between the box and 1-D models for these end-of-night concentrations of NO<sub>x</sub> and O<sub>3</sub>. This parametrisation would could also be used in global climate-chemistry models with limited vertical resolution near the surface. Box-model results for the following day differ substantially if this effective nocturnal deposition velocity for ozone is implemented; for instance, there is a 9% increase in the following days peak ozone concentration. However under medium to high [NO <sub>x</sub>] conditions (NO<sub>x</sub> &gt; 1 ppbv), the effect on the chemistry due to the vertical distribution of the species means no box model can adequately represent chemistry in the NBL without modifying reaction rate coefficients.</p>}},
  author       = {{Pugh, Thomas A.M. and Ryder, James and MacKenzie, A. Robert and Moller, Sarah J. and Lee, James D. and Helfter, Carole and Nemitz, Eiko and Lowe, Douglas and Hewitt, C. Nicholas}},
  issn         = {{0167-7764}},
  keywords     = {{Box model; NO; Nocturnal boundary-layer; Ozone; Rainforest}},
  language     = {{eng}},
  number       = {{2-3}},
  pages        = {{89--110}},
  publisher    = {{Springer}},
  series       = {{Journal of Atmospheric Chemistry}},
  title        = {{Modelling chemistry in the nocturnal boundary layer above tropical rainforest and a generalised effective nocturnal ozone deposition velocity for sub-ppbv NO<sub>x</sub> conditions}},
  url          = {{http://dx.doi.org/10.1007/s10874-011-9183-4}},
  doi          = {{10.1007/s10874-011-9183-4}},
  volume       = {{65}},
  year         = {{2010}},
}