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Aerosol water alone cannot fix organic-aerosol bias

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Adding aerosol liquid water to SOA partitioning without non-ideality overpredicts nighttime carbon; daytime OA in the southeast US still needs extra sources.

Source

On the implications of aerosol liquid water and phase separation for organic aerosol mass

Pye HOT, Murphy BN, Xu L, et al. · Atmospheric chemistry and physics · 2017

doi.org/10.5194/acp-17-343-2017Read the full paper ↗93 citationscc by

What they did

Authors updated CMAQ over the eastern United States for June 2013 (SOAS) so semivolatile SOA could interact with aerosol water, including organic-phase water uptake and a non-ideal activity-coefficient case, then compared OC with IMPROVE, CSN, and SEARCH.

What they found

The non-ideal (γ ≠ 1) case cut OC bias to −4, −10, and −2% at IMPROVE, CSN, and SEARCH. Assuming ideality overestimates nighttime aerosol water and carbon. Water-soluble OA was ~90% of total OA in the southeast US summer, but daytime OA remains underpredicted even with water in the partitioning medium.

The limits

What it doesn't show

The work is one summer over the eastern US; it does not identify the missing daytime SOA precursors, and POA is still overestimated by about a factor of two, compensating some SOA underestimate.

Key terms

SOA
Secondary organic aerosol formed from oxidation of gas-phase organics.
Aerosol liquid water
Water taken up by particles that can change size, chemistry, and partitioning.
Activity coefficient (γ)
Factor describing non-ideal mixing; γ ≠ 1 reduces water-driven SOA uptake.
WSOC
Water-soluble organic carbon, often used as a SOA/OOA surrogate.
SOAS
Southern Oxidant and Aerosol Study (2013) in the southeast United States.

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Quiz yourself

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Adding aerosol water as an ideal solvent tends to:

Common questions

Should models dump all organics into aerosol water?

No—without non-ideality, nighttime water and carbon are overestimated.

Does adding water fix daytime OA?

No; extra daytime precursors or pathways are still needed.

What fraction of southeast US OA was water-soluble in SOAS?

About 90% of total OA on average in summer 2013.

Which biogenic nitrates were least soluble?

Monoterpene nitrates, consistent with similar dry vs humid β-pinene + NO3 yields.

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