scholarly journals Chemical mass closure and assessment of the origin of the submicron aerosol in the marine boundary layer and the free troposphere at Tenerife during ACE-2

Tellus B ◽  
2000 ◽  
Vol 52 (2) ◽  
pp. 141-168 ◽  
Author(s):  
J.-P. Putaud ◽  
R. Van Dingenen ◽  
M. Mangoni ◽  
A. Virkkula ◽  
F. Raes ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Marine Boundary Layer ◽  
Free Troposphere ◽  
Mass Closure ◽  
Submicron Aerosol ◽  
Chemical Mass Closure

scholarly journals Impact of nucleation on global CCN

2009 ◽  
Vol 9 (3) ◽  
pp. 12999-13037 ◽  
Author(s):  
J. Merikanto ◽  
D. V. Spracklen ◽  
G. W. Mann ◽  
S. J. Pickering ◽  
K. S. Carslaw
Keyword(s):  
Boundary Layer ◽  
Marine Boundary Layer ◽  
Environmental Changes ◽  
Control Strategies ◽  
Cloud Condensation Nuclei ◽  
Free Troposphere ◽  
Carbonaceous Particles ◽  
Upper Troposphere ◽  
Low Level ◽  
Primary Emissions

Abstract. Cloud condensation nuclei (CCN) are derived from particles emitted directly into the atmosphere (primary emissions) or from the growth of nanometer-sized particles nucleated in the atmosphere. It is important to separate these two sources because they respond in different ways to gas and particle emission control strategies and environmental changes. Here, we use a global aerosol microphysics model to quantify the contribution of primary and nucleated particles to global CCN. The model considers primary emissions of sea spray, sulfate and carbonaceous particles, and nucleation processes appropriate for the free troposphere and boundary layer. We estimate that 45% of global low-level cloud CCN at 0.2% supersaturation are secondary aerosol derived from nucleation (ranging between 31–49% taking into account uncertainties primary emissions and nucleation rates), the remainder being directly emitted as primary aerosol. The model suggests that 35% of CCN (0.2%) in low-level clouds were created in the free and upper troposphere. In the marine boundary layer 55% of CCN (0.2%) are from nucleation, 45% being entrained from the free troposphere. Both in global and marine boundary layer 10% of CCN (0.2%) is nucleated in the boundary layer. Combinations of model runs show that primary and nucleated CCN are non-linearly coupled. In particular, boundary layer nucleated CCN are strongly suppressed by both primary emissions and entrainment of particles nucleated in the free troposphere. Elimination of all primary emissions reduces global CCN (0.2%) by only 20% and elimination of upper tropospheric nucleation reduces CCN (0.2%) by only 12% because of increased impact of boundary layer nucleation on CCN.

scholarly journals Long-Term Trends in Marine Boundary Layer Properties over the Atlantic Ocean

2019 ◽  
Vol 32 (10) ◽  
pp. 2991-3004 ◽  
Author(s):  
Juan P. Díaz ◽  
Francisco J. Expósito ◽  
Juan C. Pérez ◽  
Albano González ◽  
Yuqing Wang ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Atlantic Ocean ◽  
Marine Boundary Layer ◽  
Inversion Layer ◽  
Precipitable Water ◽  
Cloud Formation ◽  
Climate Projections ◽  
Free Troposphere ◽  
Long Term Trends

Abstract The marine boundary layer (MBL) is a key component of Earth’s climate system, and its main characteristics (height, entrainment efficiency, energy and mass fluxes, cloud formation processes, etc.) are closely linked to the properties of the inversion layer, which generally determines its height. Furthermore, cloud response to a warmer climate, one of the main sources of uncertainty in future climate projections, is highly dependent on changes in the MBL and in the inversion-layer properties. Long-term trends of the time series of MBL parameters at 32 stations in the Atlantic Ocean have been analyzed using conveniently homogenized radiosonde profiles from 1981 to 2010. In general, decreasing trends are found in the strength and thickness of the inversion layer and in the difference between the precipitable water vapor (PWV) in the free troposphere and the MBL. In contrast, positive trends are found in the height of the bottom of the inversion layer, the lapse rates of virtual and equivalent potential temperatures, the PWV within the boundary layer, and the sea surface temperature (SST). The weakening trend of the inversion layer and the increasing desiccation of the free troposphere relative to the MBL could have important consequences for both the evolution of low cloud cover in a greenhouse-warming climate and the fragile local ecosystems, such as “cloud forests.”

scholarly journals The impact of monoaromatic hydrocarbons on OH reactivity in the coastal UK boundary layer and free troposphere

2014 ◽  
Vol 14 (13) ◽  
pp. 6677-6693 ◽  
Author(s):  
R. T. Lidster ◽  
J. F. Hamilton ◽  
J. D. Lee ◽  
A. C. Lewis ◽  
J. R. Hopkins ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Gas Chromatography ◽  
Atmospheric Chemistry ◽  
Marine Boundary Layer ◽  
Ethyl Benzene ◽  
Free Troposphere ◽  
Flight Mass Spectrometry ◽  
Benzene Toluene ◽  
The Uk ◽  
The Impact

Abstract. Reaction with the hydroxyl radical (OH) is the dominant removal mechanism for virtually all volatile organic compounds (VOCs) in the atmosphere; however, it can be difficult to reconcile measured OH reactivity with known sinks. Unresolved higher molecular weight VOCs contribute to OH sinks, of which monoaromatics are potentially an important sub-class. A method based on comprehensive two-dimensional gas chromatography coupled to time-of-flight mass spectrometry (GC × GC-TOFMS) has been developed that extends the degree with which larger VOCs can be individually speciated from whole air samples (WAS). The technique showed excellent sensitivity, resolution and good agreement with an established gas chromatography–flame ionisation (GC-FID) method, for compounds amenable to analysis on both instruments. Measurements have been made of VOCs within the UK east coast marine boundary layer and free troposphere, using samples collected from five aircraft flights in winter 2011. Ten monoaromatic compounds with an array of different alkyl ring substituents have been quantified, in addition to the simple aromatics, benzene, toluene, ethyl benzene and Σm- and p-xylene. These additional compounds were then included in constrained box model simulations of atmospheric chemistry occurring at two UK rural and suburban field sites in order to assess the potential impact of these larger monoaromatics species on OH reactivity; they have been calculated to contribute an additional 2–6% to the overall modelled OH loss rate, providing a maximum additional OH sink of ~0.9 s−1.

scholarly journals Free troposphere as the dominant source of CCN in the Equatorial Pacific boundary layer: long-range transport and teleconnections

2013 ◽  
Vol 13 (1) ◽  
pp. 1279-1326 ◽  
Author(s):  
A. D. Clarke ◽  
S. Freitag ◽  
R. M. C. Simpson ◽  
J. G. Hudson ◽  
S. G. Howell ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Marine Boundary Layer ◽  
Cloud Condensation Nuclei ◽  
Large Fraction ◽  
Deep Convection ◽  
Equatorial Pacific ◽  
Quasi Equilibrium ◽  
Free Troposphere ◽  
Low Carbon ◽  
Mixing Ratios

Abstract. Airborne aerosol measurements in the central equatorial Pacific during PASE (Pacific Atmospheric Sulfur Experiment) revealed that cloud condensation nuclei (CCN) activated in marine boundary layer (MBL) clouds were dominated by entrainment from the free troposphere (FT). About 65% entered at sizes effective as CCN in MBL clouds, while 25% entered the MBL too small to activate but subsequently grew via gas to particle conversion. The remaining 10% were inferred to be sea-salt aerosol; there was no discernable nucleation in the MBL. FT aerosols at low carbon monoxide (CO) mixing ratios (< 63 ppbv) were small and relatively volatile with a number mode around 30–40 nm dry diameter and tended to be associated with cloud outflow from distant deep convection (3000 km or more). Higher CO concentrations were commonly associated with trajectories from South America and the Amazon region (ca. 10 000 km away) and occurred in layers indicative of combustion sources partially scavenged by precipitation. These had number mode near 60–80 nm diameter with a large fraction already CCN.2 (those activated at 0.2% supersaturation and representative of MBL clouds) before entrainment into the MBL. Flight averaged concentrations of CCN.2 were similar for measurements near the surface, below the inversion and above the inversion, confirming that subsidence of FT aerosol dominated MBL CCN.2. Concurrent flight-to-flight variations of CCN.2 at all altitudes below 3 km imply MBL CCN.2 concentrations were in quasi-equilibrium with the FT over a 2–3 day time scale. This extended FT transport over thousands of kilometers indicates teleconnections between MBL CCN and cloud-scavenged sources of both natural and/or residual combustion origin. The low aerosol scattering and mass in such layers results in poor detection by satellite and this source of CCN is not represented in most current models. The measurements confirm nucleation in the MBL was not evident during PASE and argue against the CLAW hypothesis being effective in this region during PASE.

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