the high-resolution version of tm5-mp for optimized satellite retrievals: description and validation
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ID: 174635
2017
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Abstract
We provide a comprehensive
description of the high-resolution version of the TM5-MP global chemistry
transport model, which is to be employed for deriving highly resolved
vertical profiles of nitrogen dioxide (NO2), formaldehyde (CH2O),
and sulfur dioxide (SO2) for use in satellite retrievals from platforms
such as the Ozone Monitoring Instrument (OMI) and the Sentinel-5 Precursor,
and the TROPOspheric Monitoring Instrument (tropOMI). Comparing simulations
conducted at horizontal resolutions of 3° × 2° and
1° × 1° reveals differences of ±20 % exist in
the global seasonal distribution of 222Rn, being larger near specific
coastal locations and tropical oceans. For tropospheric ozone (O3),
analysis of the chemical budget terms shows that the impact on globally
integrated photolysis rates is rather low, in spite of the higher spatial
variability of meteorological data fields from ERA-Interim at
1° × 1°. Surface concentrations of O3 in
high-NOx regions decrease between 5 and 10 % at
1° × 1° due to a reduction in NOx recycling
terms and an increase in the associated titration term of O3 by NO. At
1° × 1°, the net global stratosphere–troposphere
exchange of O3 decreases by ∼ 7 %, with an associated shift in
the hemispheric gradient. By comparing NO, NO2, HNO3 and
peroxy-acetyl-nitrate (PAN) profiles against measurement composites, we show
that TM5-MP captures the vertical distribution of NOx and long-lived
NOx reservoirs at background locations, again with modest changes at
1° × 1°. Comparing monthly mean distributions in
lightning NOx and applying ERA-Interim convective mass fluxes, we show
that the vertical re-distribution of lightning NOx changes with enhanced
release of NOx in the upper troposphere. We show that surface mixing
ratios in both NO and NO2 are generally underestimated in both low- and
high-NOx scenarios. For Europe, a negative bias exists for [NO] at the
surface across the whole domain, with lower biases at
1° × 1° at only ∼ 20 % of sites. For
NO2, biases are more variable, with lower (higher) biases at
1° × 1° occurring at ∼ 35 % ( ∼ 20 %)
of sites, with the remainder showing little change. For CH2O, the impact
of higher resolution on the chemical budget terms is rather modest, with
changes of less than 5 %. The simulated vertical distribution of CH2O
agrees reasonably well with measurements in pristine locations, although
column-integrated values are generally underestimated relative to satellite
measurements in polluted regions. For SO2, the performance at
1° × 1° is principally governed by the quality of
the emission inventory, with limited improvements in the site-specific
biases, with most showing no significant improvement. For the vertical
column, improvements near strong source regions occur which reduce the biases
in the integrated column. For remote regions missing biogenic source terms
are inferred.
| Reference Key |
williams2017geoscientificthe
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|---|---|
| Authors | ;J. E. Williams;K. F. Boersma;P. Le Sager;W. W. Verstraeten |
| Journal | international journal of quantum chemistry |
| Year | 2017 |
| DOI |
10.5194/gmd-10-721-2017
|
| URL | |
| Keywords |
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