Airborne observations over the Amazon Basin showed high aerosol particle concentrations in the upper troposphere (UT) between 8 and 15 km altitude, with number densities (normalized to standard ...temperature and pressure) often exceeding those in the planetary boundary layer (PBL) by 1 or 2 orders of magnitude. The measurements were made during the German–Brazilian cooperative aircraft campaign ACRIDICON–CHUVA, where ACRIDICON stands for Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems and CHUVA is the acronym for Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (global precipitation measurement), on the German High Altitude and Long Range Research Aircraft (HALO). The campaign took place in September–October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with atmospheric trace gases, aerosol particles, and atmospheric radiation. Aerosol enhancements were observed consistently on all flights during which the UT was probed, using several aerosol metrics, including condensation nuclei (CN) and cloud condensation nuclei (CCN) number concentrations and chemical species mass concentrations. The UT particles differed sharply in their chemical composition and size distribution from those in the PBL, ruling out convective transport of combustion-derived particles from the boundary layer (BL) as a source. The air in the immediate outflow of deep convective clouds was depleted of aerosol particles, whereas strongly enhanced number concentrations of small particles (< 90 nm diameter) were found in UT regions that had experienced outflow from deep convection in the preceding 5–72 h. We also found elevated concentrations of larger (> 90 nm) particles in the UT, which consisted mostly of organic matter and nitrate and were very effective CCN. Our findings suggest a conceptual model, where production of new aerosol particles takes place in the continental UT from biogenic volatile organic material brought up by deep convection and converted to condensable species in the UT. Subsequently, downward mixing and transport of upper tropospheric aerosol can be a source of particles to the PBL, where they increase in size by the condensation of biogenic volatile organic compound (BVOC) oxidation products. This may be an important source of aerosol particles for the Amazonian PBL, where aerosol nucleation and new particle formation have not been observed. We propose that this may have been the dominant process supplying secondary aerosol particles in the pristine atmosphere, making clouds the dominant control of both removal and production of atmospheric particles.
The global variability of clouds and their interactions
with aerosol and radiation make them one of our largest sources of
uncertainty related to global radiative forcing. The droplet size
...distribution (DSD) of clouds is an excellent proxy that connects cloud
microphysical properties with radiative impacts on our climate. However,
traditional radiometric instruments are information-limited in their DSD
retrievals. Radiometric sensors can infer droplet effective radius directly
but not the distribution width, which is an important parameter tied to the
growth of a cloud field and to the onset of precipitation. DSD heterogeneity
hidden inside large pixels, a lack of angular information, and the absence of
polarization limit the amount of information these retrievals can provide.
Next-generation instruments that can measure at narrow resolutions with multiple
view angles on the same pixel, a broad swath, and sensitivity to
the intensity and polarization of light are best situated to retrieve DSDs at
the pixel level and over a wide spatial field. The Airborne Hyper-Angular
Rainbow Polarimeter (HARP) is a wide-field-of-view imaging polarimeter
instrument designed by the University of Maryland, Baltimore County (UMBC),
for retrievals of cloud droplet size distribution properties over a wide
swath, at narrow resolution, and at up to 60 unique, co-located view zenith
angles in the 670 nm channel. The cloud droplet effective radius (CDR) and
variance (CDV) of a unimodal gamma size distribution are inferred
simultaneously by matching measurement to Mie polarized phase functions. For
all targets with appropriate geometry, a retrieval is possible, and
unprecedented spatial maps of CDR and CDV are made for cloud fields that
stretch both across the swath and along the entirety of a flight
observation. During the NASA Lake Michigan Ozone Study (LMOS) aircraft
campaign in May–June 2017, the Airborne HARP (AirHARP) instrument observed
a heterogeneous stratocumulus cloud field along the solar principal plane.
Our retrievals from this dataset show that cloud DSD heterogeneity can occur
at the 200 m scale, much smaller than the 1–2 km resolution of most spaceborne
sensors. This heterogeneity at the sub-pixel level can create artificial
broadening of the DSD in retrievals made at resolutions on the order of 0.5
to 1 km. This study, which uses the AirHARP instrument and its data as a
proxy for upcoming HARP CubeSat and HARP2 spaceborne instruments,
demonstrates the viability of the HARP concept to make cloud measurements at
scales of individual clouds, with global coverage, and in a low-cost,
compact CubeSat-sized payload.
The Green Ocean Amazon experiment – GoAmazon 2014–2015 – explored the interactions between natural biogenic forest emissions from central Amazonia and urban air pollution from Manaus. Previous ...GoAmazon 2014–2015 studies showed that nitrogen oxide (NOx = NO + NO2) and sulfur oxide (SOx) emissions from Manaus strongly interact with biogenic volatile organic compounds (BVOCs), affecting secondary organic aerosol (SOA) formation. In previous studies, ground-based and aircraft measurements provided evidence of SOA formation and strong changes in aerosol composition and properties. Aerosol optical properties also evolve, and their impacts on the Amazonian ecosystem can be significant. As particles age, some processes, such as SOA production, black carbon (BC) deposition, particle growth and the BC lensing effect change the aerosol optical properties, affecting the solar radiation flux at the surface. This study analyzes data and models SOA formation using the Weather Research and Forecasting with Chemistry (WRF-Chem) model to assess the spatial variability in aerosol optical properties as the Manaus plumes interact with the natural atmosphere. The following aerosol optical properties are investigated: single scattering albedo (SSA), asymmetry parameter (gaer), absorption Ångström exponent (AAE) and scattering Ångström exponent (SAE). These simulations were validated using ground-based measurements at three experimental sites, namely the Amazon Tall Tower Observatory – ATTO (T0a), downtown Manaus (T1), Tiwa Hotel (T2) and Manacapuru (T3), as well as the U.S. Department of Energy (DOE) Gulfstream 1 (G-1) aircraft flights. WRF-Chem simulations were performed over 7 d during March 2014. Results show a mean biogenic SOA (BSOA) mass enrichment of 512 % at the T1 site, 450 % in regions downwind of Manaus, such as the T3 site, and 850 % in areas north of the T3 site in simulations with anthropogenic emissions. The SOA formation is rather fast, with about 80 % of the SOA mass produced in 3–4 h. Comparing the plume from simulations with and without anthropogenic emissions, SSA shows a downwind reduction of approximately 10 %, 11 % and 6 % at the T1, T2 and T3 sites, respectively. Other regions, such as those further downwind of the T3 site, are also affected. The gaer values increased from 0.62 to 0.74 at the T1 site and from 0.67 to 0.72 at the T3 site when anthropogenic emissions are active. During the Manaus plume-aging process, a plume tracking analysis shows an increase in SSA from 0.91 close to Manaus to 0.98 160 km downwind of Manaus as a result of SOA production and BC deposition.
Quantifying the aerosol/cloud-mediated radiative effect at a global scale requires simultaneous satellite retrievals of cloud condensation nuclei (CCN) concentrations and cloud base updraft ...velocities (Wb
). Hitherto, the inability to do so has been a major cause of high uncertainty regarding anthropogenic aerosol/cloud-mediated radiative forcing. This can be addressed by the emerging capability of estimating CCN and Wb
of boundary layer convective clouds from an operational polar orbiting weather satellite. Our methodology uses such clouds as an effective analog for CCN chambers. The cloud base supersaturation (S) is determined by Wb
and the satellite-retrieved cloud base drop concentrations (Ndb
), which is the same as CCN(S). Validation against ground-based CCN instruments at Oklahoma, at Manaus, and onboard a ship in the northeast Pacific showed a retrieval accuracy of ±25% to ±30% for individual satellite overpasses. The methodology is presently limited to boundary layer not raining convective clouds of at least 1 km depth that are not obscured by upper layer clouds, including semitransparent cirrus. The limitation for small solar backscattering angles of <25° restricts the satellite coverage to ∼25% of the world area in a single day.
The climate of South America exhibits pronounced differences between rainy and dry seasons, associated with specific synoptic features such as the establishment of the South Atlantic convergence ...zone. Here, we analyze the spatiotemporal correlation structure and in particular teleconnections of daily rainfall associated with these features by means of evolving complex networks. A modification of Pearson’s correlation coefficient is introduced to handle the intricate statistical properties of daily rainfall. On this basis, spatial correlation networks are constructed, and new appropriate network measures are introduced in order to analyze the temporal evolution of the networks’ characteristics. We particularly focus on the identification of coherent areas of similar rainfall patterns and previously unknown teleconnection structures between remote areas. We show that the monsoon onset is characterized by an abrupt transition from erratic to organized regional connectivity that prevails during the monsoon season, while only the onset times themselves exhibit anomalous large-scale organization of teleconnections. Furthermore, we reveal that the two mega-droughts in the Amazon basin were already announced in the previous year by an anomalous behavior of the connectivity structure.
Cirrus clouds cover a large fraction of tropical latitudes and play an important role in Earth's radiation budget. Their optical properties, altitude, vertical and horizontal coverage control their ...radiative forcing, and hence detailed cirrus measurements at different geographical locations are of utmost importance. Studies reporting cirrus properties over tropical rain forests like the Amazon, however, are scarce. Studies with satellite profilers do not give information on the diurnal cycle, and the satellite imagers do not report on the cloud vertical structure. At the same time, ground-based lidar studies are restricted to a few case studies. In this paper, we derive the first comprehensive statistics of optical and geometrical properties of upper-tropospheric cirrus clouds in Amazonia. We used 1 year (July 2011 to June 2012) of ground-based lidar atmospheric observations north of Manaus, Brazil. This dataset was processed by an automatic cloud detection and optical properties retrieval algorithm. Upper-tropospheric cirrus clouds were observed more frequently than reported previously for tropical regions. The frequency of occurrence was found to be as high as 88 % during the wet season and not lower than 50 % during the dry season. The diurnal cycle shows a minimum around local noon and maximum during late afternoon, associated with the diurnal cycle of precipitation. The mean values of cirrus cloud top and base heights, cloud thickness, and cloud optical depth were 14.3 ± 1.9 (SD) km, 12.9 ± 2.2 km, 1.4 ± 1.1 km, and 0.25 ± 0.46, respectively. Cirrus clouds were found at temperatures down to −90 °C. Frequently cirrus were observed within the tropical tropopause layer (TTL), which are likely associated to slow mesoscale uplifting or to the remnants of overshooting convection. The vertical distribution was not uniform, and thin and subvisible cirrus occurred more frequently closer to the tropopause. The mean lidar ratio was 23.3 ± 8.0 sr. However, for subvisible cirrus clouds a bimodal distribution with a secondary peak at about 44 sr was found suggesting a mixed composition. A dependence of the lidar ratio with cloud temperature (altitude) was not found, indicating that the clouds are vertically well mixed. The frequency of occurrence of cirrus clouds classified as subvisible (τ < 0. 03) were 41.6 %, whilst 37.8 % were thin cirrus (0. 03 < τ < 0. 3) and 20.5 % opaque cirrus (τ > 0. 3). Hence, in central Amazonia not only a high frequency of cirrus clouds occurs, but also a large fraction of subvisible cirrus clouds. This high frequency of subvisible cirrus clouds may contaminate aerosol optical depth measured by sun photometers and satellite sensors to an unknown extent.
Multi-angle polarimetric (MAP) imaging of Earth scenes can be used for the retrieval of microphysical and optical parameters of aerosols and clouds. The Airborne Hyper-Angular Rainbow Polarimeter ...(AirHARP) is an aircraft MAP instrument with a hyper-angular imaging capability of 60 along-track viewing angles at 670 nm and 20 along-track viewing angles at other wavelengths – 440, 550, and 870 nm – across the full 114∘ (94∘) along-track (cross-track) field of view. Here we report the retrieval of aerosol properties using the Generalized Retrieval of Aerosols and Surface Properties (GRASP) algorithm applied to AirHARP observations collected during the NASA Aerosol Characterization from Polarimeter and Lidar (ACEPOL) campaign in October–November 2017. The retrieved aerosol properties include spherical fraction (SF), aerosol column concentration in multiple size distribution modes, and, with sufficient aerosol loading, complex aerosol refractive index. From these primary retrievals, we derive aerosol optical depth (AOD), Angstrom exponent (AE), and single scattering albedo (SSA). AODs retrieved from AirHARP measurements are compared with the High Spectral Resolution LiDAR-2 (HSRL2) AOD measurements at 532 nm and validated with measurements from collocated Aerosol Robotic NETwork (AERONET) stations. A good agreement with HSRL2 (ρ=0.940, |BIAS|=0.062, mean absolute error (MAE) = 0.122) and AERONET AOD (0.010≤MAE≤0.015, 0.002≤|BIAS|≤0.009) measurements is observed for the collocated points. There was a mismatch between the HSRL2- and AirHARP-retrieved AOD for the pixels close to the forest fire smoke source and to the edges of the plume due to spatial mismatch in the sampling. This resulted in a higher BIAS and MAE for the HSRL2 AOD comparison. For the case of AERONET AOD comparison, two different approaches are used in the GRASP retrievals, and the simplified aerosol component-based GRASP/Models kernel which retrieves fewer number of aerosol parameter performed well compared to a more generous GRASP/Five mode approach in the low aerosol loading cases. Forest fire smoke intercepted during ACEPOL provided a situation with homogenous plume and sufficient aerosol loading to retrieve the real part of the refractive index (RRI) of 1.55 and the imaginary part of the refractive index (IRI) of 0.024. The derived SSAs for this case are 0.87, 0.86, 0.84, and 0.81 at wavelengths of 440, 550, 670, and 870 nm, respectively. Finer particles with an average AE of 1.53, a volume median radius of 0.157 µm, and a standard deviation (SD) of 0.55 for fine mode is observed for the same smoke plume. These results serve as a proxy for the scale and detail of aerosol retrievals that are anticipated from future space mission data, as HARP CubeSat (mission begins 2020) and HARP2 (aboard the NASA PACE mission with launch in 2023) are near duplicates of AirHARP and are expected to provide the same level of aerosol characterization.
The effects of aerosol particles and updraft speed on warm-phase cloud microphysical properties are studied in the Amazon region as part of the ACRIDICON-CHUVA experiment. Here we expand the ...sensitivity analysis usually found in the literature by concomitantly considering cloud evolution, putting the sensitivity quantifications into perspective in relation to in-cloud processing, and by considering the effects on droplet size distribution (DSD) shape. Our in situ aircraft measurements over the Amazon Basin cover a wide range of particle concentration and thermodynamic conditions, from the pristine regions over coastal and forested areas to the southern Amazon, which is highly polluted from biomass burning. The quantitative results show that particle concentration is the primary driver for the vertical profiles of effective diameter and droplet concentration in the warm phase of Amazonian convective clouds, while updraft speeds have a modulating role in the latter and in total condensed water. The cloud microphysical properties were found to be highly variable with altitude above cloud base, which we used as a proxy for cloud evolution since it is a measure of the time droplets that were subject to cloud processing. We show that DSD shape is crucial in understanding cloud sensitivities. The aerosol effect on DSD shape was found to vary with altitude, which can help models to better constrain the indirect aerosol effect on climate.
During the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) campaign, size-resolved cloud condensation nuclei (CCN) spectra were characterized at a research site (T3) 60 km ...downwind of the city of Manaus, Brazil, in central Amazonia for 1 year (12 March 2014 to 3 March 2015). Particle hygroscopicity (κCCN) and mixing state were derived from the size-resolved CCN spectra, and the hygroscopicity of the organic component of the aerosol (κorg) was then calculated from κCCN and concurrent chemical composition measurements. The annual average κCCN increased from 0.13 at 75 nm to 0.17 at 171 nm, and the increase was largely due to an increase in sulfate volume fraction. During both wet and dry seasons, κCCN, κorg, and particle composition under background conditions exhibited essentially no diel variations. The constant κorg of ∼ 0. 15 is consistent with the largely uniform and high O : C value (∼ 0. 8), indicating that the aerosols under background conditions are dominated by the aged regional aerosol particles consisting of highly oxygenated organic compounds. For air masses strongly influenced by urban pollution and/or local biomass burning, lower values of κorg and organic O : C atomic ratio were observed during night, due to accumulation of freshly emitted particles, dominated by primary organic aerosol (POA) with low hygroscopicity, within a shallow nocturnal boundary layer. The O : C, κorg, and κCCN increased from the early morning hours and peaked around noon, driven by the formation and aging of secondary organic aerosol (SOA) and dilution of POA emissions into a deeper boundary layer, while the development of the boundary layer, which leads to mixing with aged particles from the residual layer aloft, likely also contributed to the increases. The hygroscopicities associated with individual organic factors, derived from PMF (positive matrix factorization) analysis of AMS (aerosol mass spectrometry) spectra, were estimated through multivariable linear regression. For the SOA factors, the variation of the κ value with O : C agrees well with the linear relationship reported from earlier laboratory studies of SOA hygroscopicity. On the other hand, the variation in O : C of ambient aerosol organics is largely driven by the variation in the volume fractions of POA and SOA factors, which have very different O : C values. As POA factors have hygroscopicity values well below the linear relationship between SOA hygroscopicity and O : C, mixtures with different POA and SOA fractions exhibit a steeper slope for the increase in κorg with O : C, as observed during this and earlier field studies. This finding helps better understand and reconcile the differences in the relationships between κorg and O : C observed in laboratory and field studies, therefore providing a basis for improved parameterization in global models, especially in a tropical context.
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