During the CARRIBA (Cloud, Aerosol, Radiation and tuRbulence in the trade wInd regime over BArbados) campaign, the interaction between aerosol particles and cloud microphysical properties was ...investigated in detail, which also includes the influence of clouds on the aerosol formation. During two intensive campaigns in 2010 and 2011, helicopter-borne measurement flights were performed to investigate the thermodynamic, turbulent, microphysical, and radiative properties of trade-wind cumuli over Barbados. During these flights, 91 cases with increased aerosol particle number concentrations near clouds were detected. The majority of these cases are also correlated with enhanced irradiance in the ultraviolet (UV) spectral wavelength range. This enhancement reaches values up to a factor of 3.3 greater compared to background values. Thus, cloud boundaries provide a perfect environment for the production of precursor gases for new particle formation. Another feature of cloud edges is an increased turbulence, which may also enhance nucleation and particle growth. The observed events have a mean length of 100 m, corresponding to a lifetime of less than 300 s. This implies that particles with diameters of at least 7 nm grew several nanometers per minute, which corresponds to the upper end of values in the literature (Kulmala et al., 2004). Such high values cannot be explained by sulfuric acid alone; thus extremely low volatility organic compounds (ELVOCs) are probably involved here.
Ice particle activation and evolution have important atmospheric implications for cloud formation, initiation of precipitation and radiative interactions. The initial formation of atmospheric ice by ...heterogeneous ice nucleation requires the presence of a nucleating seed, an ice-nucleating particle (INP), to facilitate its first emergence. Unfortunately, only a few long-term measurements of INPs exist, and as a result, knowledge about geographic and seasonal variations of INP concentrations is sparse. Here we present data from nearly 2 years of INP measurements from four stations in different regions of the world: the Amazon (Brazil), the Caribbean (Martinique), central Europe (Germany) and the Arctic (Svalbard). The sites feature diverse geographical climates and ecosystems that are associated with dissimilar transport patterns, aerosol characteristics and levels of anthropogenic impact (ranging from near pristine to mostly rural). Interestingly, observed INP concentrations, which represent measurements in the deposition and condensation freezing modes, do not differ greatly from site to site but usually fall well within the same order of magnitude. Moreover, short-term variability overwhelms all long-term trends and/or seasonality in the INP concentration at all locations. An analysis of the frequency distributions of INP concentrations suggests that INPs tend to be well mixed and reflective of large-scale air mass movements. No universal physical or chemical parameter could be identified to be a causal link driving INP climatology, highlighting the complex nature of the ice nucleation process. Amazonian INP concentrations were mostly unaffected by the biomass burning season, even though aerosol concentrations increase by a factor of 10 from the wet to dry season. Caribbean INPs were positively correlated to parameters related to transported mineral dust, which is known to increase during the Northern Hemisphere summer. A wind sector analysis revealed the absence of an anthropogenic impact on average INP concentrations at the site in central Europe. Likewise, no Arctic haze influence was observed on INPs at the Arctic site, where low concentrations were generally measured. We consider the collected data to be a unique resource for the community that illustrates some of the challenges and knowledge gaps of the field in general, while specifically highlighting the need for more long-term observations of INPs worldwide.
Abstract
The atmospheric oxidation of biogenic volatile organic compounds (BVOC) by OH radicals over tropical rainforests impacts local particle production and the lifetime of globally distributed ...chemically and radiatively active gases. For the pristine Amazon rainforest during the dry season, we empirically determined the diurnal OH radical variability at the forest-atmosphere interface region between 80 and 325 m from 07:00 to 15:00 LT using BVOC measurements. A dynamic time warping approach was applied showing that median averaged mixing times between 80 to 325 m decrease from 105 to 15 min over this time period. The inferred OH concentrations show evidence for an early morning OH peak (07:00–08:00 LT) and an OH maximum (14:00 LT) reaching 2.2 (0.2, 3.8) × 10
6
molecules cm
−3
controlled by the coupling between BVOC emission fluxes, nocturnal NO
x
accumulation, convective turbulence, air chemistry and photolysis rates. The results were evaluated with a turbulence resolving transport (DALES), a regional scale (WRF-Chem) and a global (EMAC) atmospheric chemistry model.
This work presents a unique combination of aerosol, cloud microphysical, thermodynamic and turbulence variables to characterize supersaturation fluctuations in a turbulent marine stratocumulus (SC) ...layer. The analysis is based on observations with the helicopter-borne measurement platform ACTOS and a detailed cloud microphysical parcel model following three different approaches: (1) From the comparison of aerosol number size distributions inside and below the SC layer, the number of activated particles is calculated as 435±87 cm−3 and compares well with the observed median droplet number concentration of Nd = 464 cm−3. Furthermore, a 50% activation diameter of Dp50≈115 nm was derived, which was linked to a critical supersaturation Scrit of 0.16% via Köhler theory. From the shape of the fraction of activated particles, we estimated a standard deviation of supersaturation fluctuations of σS' = 0.09%. (2) These estimates are compared to more direct thermodynamic observations at cloud base. Therefore, supersaturation fluctuations (S') are calculated based on highly-resolved thermodynamic data showing a standard deviation of S' ranging within 0.1%≤σS'≤0.3 %. (3) The sensitivity of the supersaturation on observed vertical wind velocity fluctuations is investigated with the help of a detailed cloud microphysical model. These results show highest fluctuations of S' with σS'=0.1% at cloud base and a decreasing σS' with increasing liquid water content and droplet number concentration. All three approaches are independent of each other and vary only within a factor of about two.
The CARRIBA (Cloud, Aerosol, Radiation and tuRbulence in the trade wInd regime over BArbados) project, focused on high resolution and collocated measurements of thermodynamic, turbulent, ...microphysical, and radiative properties of trade wind cumuli over Barbados, is introduced. The project is based on two one-month field campaigns in November 2010 (climatic wet season) and April 2011 (climatic dry season). Observations are based on helicopter-borne and ground-based measurements in an area of 100 km2 off the coast of Barbados. CARRIBA is accompanied by long-term observations at the Barbados Cloud Observatory located at the East coast of Barbados since early in 2010 and which provides a longer-term context for the CARRIBA measurements. The deployed instrumentation and sampling strategy are presented together with a classification of the meteorological conditions. The two campaigns were influenced by different air masses advected from the Caribbean area, the Atlantic Ocean, and the African continent which led to distinct aerosol conditions. Pristine conditions with low aerosol particle number concentrations of ~100 cm3 were alternating with periods influenced by Saharan dust or aerosol from biomass burning resulting in comparably high number concentrations of ~ 500 cm3. The biomass burning aerosol was originating from both the Caribbean area and Africa. The shallow cumulus clouds responded to the different aerosol conditions with a wide range of mean droplet sizes and number concentrations. Two days with different aerosol and cloud microphysical properties but almost identical meteorological conditions have been analyzed in detail. The differences in the droplet number concentration and droplet sizes appear not to show any significant change for turbulent cloud mixing, but the relative roles of droplet inertia and sedimentation in initiating coalescence, as well as the cloud reflectivity, do change substantially.
Aerosol particle measurements in the atmospheric boundary layer performed by a helicopter-borne measurement payload and by a lidar system from a case study during the IMPACT field campaign in Cabauw ...(NL) are presented. Layers of increased number concentrations of ultrafine particles were observed in the residual layer, indicating relatively recent new-particle formation. These layers were characterized by a sub-critical Richardson number and concomitant increased turbulence. Turbulent mixing is likely to lead to local supersaturation of possible precursor gases which are essential for new particle formation. Observed peaks in the number concentrations of ultrafine particles at ground level are connected to the new particle formation in the residual layer by boundary layer development and vertical mixing.
Clear experimental evidence of the Twomey effect for shallow trade wind cumuli near Barbados is presented. Effective droplet radius (reff) and cloud optical thickness (τ), retrieved from ...helicopter‐borne spectral cloud‐reflected radiance measurements, and spectral cloud reflectivity (γλ) are correlated with collocated in situ observations of the number concentration of aerosol particles from the subcloud layer (N). N denotes the concentration of particles larger than 80 nm in diameter and represents particles in the activation mode. In situ cloud microphysical and aerosol parameters were sampled by the Airborne Cloud Turbulence Observation System (ACTOS). Spectral cloud‐reflected radiance data were collected by the Spectral Modular Airborne Radiation measurement sysTem (SMART‐HELIOS). With increasing N a shift in the probability density functions of τ and γλ toward larger values is observed, while the mean values and observed ranges of retrieved reff decrease. The relative susceptibilities (RS) of reff, τ, and γλ to N are derived for bins of constant liquid water path. The resulting values of RS are in the range of 0.35 for reff and τ, and 0.27 for γλ. These results are close to the maximum susceptibility possible from theory. Overall, the shallow cumuli sampled near Barbados show characteristics of homogeneous, plane‐parallel clouds. Comparisons of RS derived from in situ measured reff and from a microphysical parcel model are in close agreement.
Key Points
Experimental evidence of Twomey effect
Susceptibility is quantified
Susceptibility of shallow cumuli shows characteristics of homogeneous clouds
A new Fast CPC (FCPC) using butanol as working fluid has been built based on the setup described by Wang et al. (2002). In this study, we describe the new instrument. The functionality and stable ...operation of the FCPC in the laboratory, as well as under atmospheric conditions, is demonstrated. The counting efficiency was measured for three temperature differences between FCPC saturator and condenser, 25, 27, and 29 K, subsequently resulting in a lower detection limit between 6.1 and 8.5 nm. Above 25 nm the FCPC reached 98–100% counting efficiency compared to an electrometer used as the reference instrument. The FCPC demonstrated its ability to perform continuous measurements over a few hours in the laboratory with respect to the total particle counting. The instrument has been implemented into the airborne measurement platform ACTOS to perform measurements in the atmospheric boundary layer. Therefore, a stable operation over two hours is required. The mixing time of the new FCPC was estimated in two ways using a time series with highly fluctuating particle number concentrations. The analysis of a sharp ramp due to a concentration change results in a mixing time of 5 ms while a spectral analysis of atmospheric data demonstrates that for frequencies up to 10 Hz coherent structures can be resolved before sampling noise dominates.
The frequency and intensity of new particle formation
(NPF) over remote forest regions in the temperate and boreal zones, and thus
the importance of NPF for the aerosol budget and life cycle in the ...pristine
atmosphere, remains controversial. Whereas NPF has been shown to occur
relatively frequently at several sites in Scandinavia, it was found to be
nearly absent at a mid-continental site in Siberia. To explore this issue
further, we made measurements of aerosol size distributions between 10 and
420 nm diameter at two remote sites in the transition region between
temperate and boreal forest in British Columbia, Canada. The measurements
covered 23 d during the month of June 2019, at the time when NPF
typically reaches its seasonal maximum in remote midlatitude regions. These
are the first such measurements in a near-pristine region on the North
American continent. Although the sites were only 150 km apart, there were
clear differences in NPF frequency and intensity between them. At the Eagle
Lake site, NPF occurred daily, and nucleation-mode particle concentrations
reached above 5000 cm−3. In contrast, at the Nazko River site, there
were only six NPF events in 11 d, and the nucleation-mode particle
concentrations only reached about 800 cm−3. The reasons for this
difference could not be conclusively resolved with the available data; they
may include air mass origins, preexisting aerosols, and the density and type
of forest cover in the surrounding regions. In contrast to observations in
other temperate and boreal environments, we found that NPF at our sites occurred
at nighttime just as frequently as during daytime. Together with the lack of
identifiable sources of sulfuric acid precursor species in the fetch
region of our sites, this suggests that nucleation of
extremely low volatility organics was the predominant NPF mechanism. Our
results indicate that extended measurement campaigns with a more
comprehensive set of instrumentation to investigate the role of NPF in the remote forest regions of North
America are essential for a deeper scientific
understanding of this important process and its role in the global aerosol
budget.
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