Identification

Title

Detailed comparisons of airborne formaldehyde measurements with box models during the 2006 INTEX-B and MILAGRO campaigns: Potential evidence for significant impacts of unmeasured and multi-generation volatile organic carbon compounds

Abstract

Detailed comparisons of airborne CH₂O measurements acquired by tunable diode laser absorption spectroscopy with steady state box model calculations were carried out using data from the 2006 INTEX-B and MILARGO campaign in order to improve our understanding of hydrocarbon oxidation processing. This study includes comparisons over Mexico (including Mexico City), the Gulf of Mexico, parts of the continental United States near the Gulf coast, as well as the more remote Pacific Ocean, and focuses on comparisons in the boundary layer. Select previous comparisons in other campaigns have highlighted some locations in the boundary layer where steady state box models have tended to underpredict CH₂O, suggesting that standard steady state modeling assumptions might be unsuitable under these conditions, and pointing to a possible role for unmeasured hydrocarbons and/or additional primary emission sources of CH₂O. Employing an improved instrument, more detailed measurement-model comparisons with better temporal overlap, up-to-date measurement and model precision estimates, up-to-date rate constants, and additional modeling tools based on both Lagrangian and Master Chemical Mechanism (MCM) runs, we have explained much of the disagreement between observed and predicted CH₂O as resulting from non-steady-state atmospheric conditions in the vicinity of large pollution sources, and have quantified the disagreement as a function of plume lifetime (processing time). We show that in the near field (within ~4 to 6 h of the source), steady-state models can either over-or-underestimate observations, depending on the predominant non-steady-state influence. In addition, we show that even far field processes (10-40 h) can be influenced by non-steady-state conditions which can be responsible for CH₂O model underestimations by ~20%. At the longer processing times in the 10 to 40 h range during Mexico City outflow events, MCM model calculations, using assumptions about initial amounts of high-order NMHCs, further indicate the potential importance of CH₂O produced from unmeasured and multi-generation hydrocarbon oxidation compounds, particularly methylglyoxal, 3-hydroxypropanal, and butan-3-one-al.

Resource type

document

Resource locator

Unique resource identifier

code

http://n2t.net/ark:/85065/d7s46t9w

codeSpace

Dataset language

eng

Spatial reference system

code identifying the spatial reference system

Classification of spatial data and services

Topic category

geoscientificInformation

Keywords

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keyword value

Text

originating controlled vocabulary

title

Resource Type

reference date

date type

publication

effective date

2016-01-01T00:00:00Z

Geographic location

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Temporal reference

Temporal extent

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Dataset reference date

date type

publication

effective date

2011-11-30T00:00:00Z

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Conformity

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Use constraints

Limitations on public access

None

Responsible organisations

Responsible party

contact position

OpenSky Support

organisation name

UCAR/NCAR - Library

full postal address

PO Box 3000

Boulder

80307-3000

email address

opensky@ucar.edu

web address

http://opensky.ucar.edu/

name: homepage

responsible party role

pointOfContact

Metadata on metadata

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