Characterisation of a new Fast CPC and its application for atmospheric particle measurements

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

Aerosols-cloud microphysics-thermodynamics-turbulence: Evaluating supersaturation in a marine stratocumulus cloud

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

Infrequent new particle formation over the remote boreal forest of Siberia

Aerosol particle number size distributions (PNSD) were investigated to verify, if extremely low-volatility organic vapors (ELVOC) from natural sources alone could induce new particle formation and growth events over the remote boreal forest region of Siberia, hundreds of kilometers away from significant anthropogenic sources. We re-evaluated observations determined at a height of 300 m of the remote observatory ZOTTO (Zotino Tall Tower Observatory, http://www.zottoproject.org). We found that new particle formation events occurred only on 11 days in a 3-year period, suggesting that homogeneous nucleation with a subsequent condensational growth could not be the major process, maintaining the particle number concentration in the planetary boundary layer of the remote boreal forest area of Siberia. © 2018 Elsevier Lt

Aerosols-cloud microphysics-thermodynamics-turbulence: Evaluating supersaturation in a marine stratocumulus cloud

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 N̄ d = 464 cm -3. Furthermore, a 50% activation diameter of D p50 ≈ 115 nm was derived, which was linked to a critical supersaturation S crit of 0.16% via Köhler theory. From the shape of the fraction of activated particles, we estimated a standard deviation of supersaturation fluctuations of σ S′ = 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%≤ σ S′ ≤ 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 σ S′ with σ S′ =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

Relationships between submicrometer particulate air pollution and air mass history in Beijing, China, 2004–2006

The Chinese capital Beijing is one of the global megacities where the effects of rapid economic growth have led to complex air pollution problems that are not well understood. In this study, ambient particle number size distributions in Beijing between 2004 and 2006 are analysed as a function of regional meteorological transport. An essential result is that the particle size distribution in Beijing depends to large extent on the history of the synoptic scale air masses. A first approach based on manual back trajectory classification yielded differences in particulate matter mass concentration by a factor of two between four different air mass categories, including three main wind directions plus the case of stagnant air masses. A back trajectory cluster analysis refined these results, yielding a total of six trajectory clusters. Besides the large scale wind direction, the transportation speed of an air mass was found to play an essential role on the PM concentrations in Beijing. Slow-moving air masses were shown to be associated with an effective accumulation of surface-based anthropogenic emissions due to both, an increased residence time over densely populated land, and their higher degree of vertical stability. For the six back trajectory clusters, differences in PM1 mass concentrations by a factor of 3.5, in the mean air mass speed by a factor of 6, and in atmospheric visibility by a factor of 4 were found. The main conclusion is that the air quality in Beijing is not only degraded by anthropogenic aerosol sources from within the megacity, but also by sources across the entire Northwest China plain depending on the meteorological situation

Observations of new particle formation in enhanced UV irradiance zones near cumulus clouds

During the CARRIBA (Cloud, Aerosol, Radiation and tuRbulence in the trade wInd regime over BArba-dos) 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.Peer reviewe

Observations of turbulence-induced new particle formation in the residual layer

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

How weather events modify aerosol particle size distributions in the Amazon boundary layer

This study evaluates the effect of weather events on the aerosol particle size distribution (PSD) at the Amazon Tall Tower Observatory (ATTO). This research combines in situ measurements of PSD and remote sensing data of lightning density, brightness temperature, cloud top height, cloud liquid water, and rain rate and vertical velocity. Measurements were obtained by scanning mobility particle sizers (SMPSs), the new generation of GOES satellites (GOES-16), the SIPAM S-band radar and the LAP 3000 radar wind profiler recently installed at the ATTO-Campina site. The combined data allow exploring changes in PSD due to different meteorological processes. The average diurnal cycle shows a higher abundance of ultrafine particles (NUFP) in the early morning, which is coupled with relatively lower concentrations in Aitken (NAIT) and accumulation (NACC) mode particles. From the early morning to the middle of the afternoon, an inverse behavior is observed, where NUFP decreases and NAIT and NACC increase, reflecting a typical particle growth process. Composite figures show an increase of NUFP before, during and after lightning was detected by the satellite above ATTO. These findings strongly indicate a close relationship between vertical transport and deep convective clouds. Lightning density is connected to a large increase in NUFP, beginning approximately 100 min before the maximum lightning density and reaching peak values around 200 min later. In addition, the removal of NACC by convective transport was found. Both the increase in NUFP and the decrease in NACC appear in parallel with the increasing intensity of lightning activity. The NUFP increases exponentially with the thunderstorm intensity. In contrast, NAIT and NACC show a different behavior, decreasing from approximately 100 min before the maximum lightning activity and reaching a minimum at the time of maximum lightning activity. The effect of cloud top height, cloud liquid water and rain rate shows the same behavior, but with different patterns between seasons. The convective processes do not occur continually but are probably modulated by gravity waves in the range of 1 to 5 h, creating a complex mechanism of interaction with a succession of updrafts and downdrafts, clouds, and clear-sky situations. The radar wind profiler measured the vertical distribution of the vertical velocity. These profiles show that downdrafts are mainly located below 10 km, while aircraft observations during the ACRIDICON–CHUVA campaign had shown maximum concentrations of ultrafine particles mainly above 10 km. Our study opens new scientific questions to be evaluated in order to understand the intricate physical and chemical mechanisms involved in the production of new particles in Amazonia.</p

The fine-scale structure of the trade wind cumuli over Barbados – An introduction to the CARRIBA project

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

Optical properties of aerosol particles over the Amazon rain forest: From background to biomass burning conditions

Atmospheric aerosols over the Amazon rainforest are strongly influenced by biomass burning activities in the southern regions of the Amazon Basin between July and October. This implies a complete change of the physical and chemical aerosol properties from the wet season, which is dominated by Primary Biological Aerosol Particles (PBAP) and biogenic secondary organic aerosols. Biomass burning emissions are highly loaded with light-absorbing aerosols, like black and brown carbon (BC and BrC, respectively). The latter one consists of a fraction of organic carbon that is able to absorb visible radiation (Andreae and Gelencs\ue9r, 2006). BrC is a strong absorber at near-UV to UV wavelengths. Therefore, light absorption by this component is wavelength dependent. This wavelength dependency, expressed as the absorption \uc5ngstr\uf6m exponent (AAE), has been used as a parameter to estimate the influence of biomass burning aerosols to total aerosol light absorption. However, the biogenic BrC contribution remains to be studied and could be significant under pristine conditions. The measurements presented here were carried out at the Amazon Tall Tower Observatory (ATTO), located 150 km NE of the city of Manaus, in the Uatum\ue3 Sustainable Development Reserve in Amazonas State, Brazil. The aerosol inlet (60 m high, 2.5 cm diameter) is installed on an 81-m triangular mast. The measurement period, from June to September 2014, includes the wetto- dry transition season (June-July) and part of the dry season (August and beginning of September). The optical properties were measured online by different instruments: 3-wavelengths nephelometer, Multi-Angle Absorption Photometer (MAAP), Single Particle Soot Photometer (SP2) and a 7-wavelength Aethalometer. Additionally, MAAP filter samples were analyzed by the Multi-Wavelength Absorbance Analyzer (MWAA) (Massab\uf2 et al, 2013), as well as levoglucosan analysis was carried out for filters collected between 18-22 August 2014. The average light absorption coefficient at 637 nm was 1.0 \ub1 0.6 Mm-1 and 5.5 \ub1 3.9 Mm-1, during the wet-to-dry transition and the dry season, respectively. Here we concentrate on measurements during 18-22 August 2014 (Figure 1) when a high absorption coefficient was measured at 637 nm, averaging 10 \ub1 3 Mm-1. The AAE calculated from MWAA measurements increased from less than 1.0 to values higher than 1.4, indicating the presence of BrC aerosol particles. This period is characterized by a long-range transport of biomass burning aerosol (confirmed by backward trajectory analysis). Levoglucosan analysis reveals significantly increased concentration but is still relatively low compared to measurements close to the source (Graham et al, 2002). Nevertheless, AAE and levoglucosan concentration show a significant correlation (r\ub2 &gt; 0.9)