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"Aerosol properties"
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Beijing Climate Center Earth System Model version 1 (BCC-ESM1): model description and evaluation of aerosol simulations
2020
The Beijing Climate Center Earth System Model version 1 (BCC-ESM1) is the first version of a fully coupled Earth system model with interactive atmospheric chemistry and aerosols developed by the Beijing Climate Center, China Meteorological Administration. Major aerosol species (including sulfate, organic carbon, black carbon, dust, and sea salt) and greenhouse gases are interactively simulated with a whole panoply of processes controlling emission, transport, gas-phase chemical reactions, secondary aerosol formation, gravitational settling, dry deposition, and wet scavenging by clouds and precipitation. Effects of aerosols on radiation, cloud, and precipitation are fully treated. The performance of BCC-ESM1 in simulating aerosols and their optical properties is comprehensively evaluated as required by the Aerosol Chemistry Model Intercomparison Project (AerChemMIP), covering the preindustrial mean state and time evolution from 1850 to 2014. The simulated aerosols from BCC-ESM1 are quite coherent with Coupled Model Intercomparison Project Phase 5 (CMIP5)-recommended data, in situ measurements from surface networks (such as IMPROVE in the US and EMEP in Europe), and aircraft observations. A comparison of modeled aerosol optical depth (AOD) at 550 nm with satellite observations retrieved from the Moderate Resolution Imaging Spectroradiometer (MODIS) and the Multi-angle Imaging SpectroRadiometer (MISR) and surface AOD observations from the AErosol RObotic NETwork (AERONET) shows reasonable agreement between simulated and observed AOD. However, BCC-ESM1 shows weaker upward transport of aerosols from the surface to the middle and upper troposphere, likely reflecting the deficiency of representing deep convective transport of chemical species in BCC-ESM1. With an overall good agreement between BCC-ESM1 simulated and observed aerosol properties, it demonstrates a success of the implementation of interactive aerosol and atmospheric chemistry in BCC-ESM1.
Journal Article
Validation of GRASP algorithm product from POLDER/PARASOL data and assessment of multi-angular polarimetry potential for aerosol monitoring
2020
Proven by multiple theoretical and practical studies,
multi-angular spectral polarimetry is ideal for comprehensive retrieval of
properties of aerosols. Furthermore, a large number of advanced space
polarimeters have been launched recently or planned to be deployed in the
coming few years (Dubovik et al.,
2019). Nevertheless, at present, practical utilization of aerosol products
from polarimetry is rather limited, due to the relatively small number of
polarimetric compared to photometric observations, as well as challenges in
making full use of the extensive information content available in these
complex observations. Indeed, while in recent years several new algorithms
have been developed to provide enhanced aerosol retrievals from satellite
polarimetry, the practical value of available aerosol products from
polarimeters yet remains to be proven. In this regard, this paper presents
the analysis of aerosol products obtained by the Generalized Retrieval of
Atmosphere and Surface Properties (GRASP) algorithm from POLDER/PARASOL
observations. After about a decade of development, GRASP has been adapted
for operational processing of polarimetric satellite observations and
several aerosol products from POLDER/PARASOL observations have been
released. These updated PARASOL/GRASP products are publicly available (e.g.,
http://www.icare.univ-lille.fr, last access: 16 October 2018, http://www.grasp-open.com/products/, last access: 28 March 2020); the dataset used in the current study is
registered under https://doi.org/10.5281/zenodo.3887265 (Chen
et al., 2020). The objective of this study is to comprehensively evaluate the GRASP aerosol
products obtained from POLDER/PARASOL observations. First, the validation of
the entire 2005–2013 archive was conducted by comparing to ground-based
Aerosol Robotic Network (AERONET) data. The subjects of the validation are
spectral aerosol optical depth (AOD), aerosol absorption optical depth
(AAOD) and single-scattering albedo (SSA) at six wavelengths, as well as
Ångström exponent (AE), fine-mode AOD (AODF) and coarse-mode AOD
(AODC) interpolated to the reference wavelength 550 nm. Second, an
inter-comparison of PARASOL/GRASP products with the PARASOL/Operational,
MODIS Dark Target (DT), Deep Blue (DB) and Multi-Angle Implementation of
Atmospheric Correction (MAIAC) aerosol products for the year 2008 was
performed. Over land both satellite data validations and inter-comparisons
were conducted separately for different surface types, discriminated by bins
of normalized difference vegetation index (NDVI): < 0.2, 0.2 ≤
and < 0.4, 0.4 ≤ and < 0.6, and ≥ 0.6. Three
PARASOL/GRASP products were analyzed: GRASP/HP (“High Precision”),
Optimized and Models. These different products are consistent but were
obtained using different assumptions in aerosol modeling with different
accuracies of atmospheric radiative transfer (RT) calculations.
Specifically, when using GRASP/HP or Optimized there is direct retrieval of
the aerosol size distribution and spectral complex index of refraction. When
using GRASP/Models, the aerosol is approximated by a mixture of several
prescribed aerosol components, each with their own fixed size distribution
and optical properties, and only the concentrations of those components are
retrieved. GRASP/HP employs the most accurate RT calculations, while
GRASP/Optimized and GRASP/Models are optimized to achieve the best trade-off
between accuracy and speed. In all these three options, the underlying
surface reflectance is retrieved simultaneously with the aerosol properties,
and the radiative transfer calculations are performed “online” during the
retrieval. All validation results obtained for the full archive of PARASOL/GRASP
products show solid quality of retrieved aerosol characteristics. The
GRASP/Models retrievals, however, provided the most solid AOD products, e.g.,
AOD (550 nm) is unbiased and has the highest correlation (R ∼ 0.92) and the highest fraction of retrievals (∼ 55.3 %)
satisfying the accuracy requirements of the Global Climate Observing System
(GCOS) when compared to AERONET observations. GRASP/HP and GRASP/Optimized
AOD products show a non-negligible positive bias (∼ 0.07) when
AOD is low (< 0.2). On the other hand, the detailed aerosol
microphysical characteristics (AE, AODF, AODC, SSA, etc.) provided by
GRASP/HP and GRASP/Optimized correlate generally better with AERONET than do
the results of GRASP/Models. Overall, GRASP/HP processing demonstrates the
high quality of microphysical characteristics retrieval versus AERONET.
Evidently, the GRASP/Models approach is more adapted for retrieval of total AOD,
while the detailed aerosol microphysical properties are limited when a
mixture of aerosol models with fixed optical properties are used. The results of a comparative analysis of PARASOL/GRASP and MODIS products
showed that, based on validation against AERONET, the PARASOL/GRASP AOD (550 nm) product is of similar and sometimes of higher quality compared to the
MODIS products. All AOD retrievals are more accurate and in good agreement
over ocean. Over land, especially over bright surfaces, the retrieval
quality degrades and the differences in total AOD products increase. The
detailed aerosol characteristics, such as AE, AODF and AODC from
PARASOL/GRASP, are generally more reliable, especially over land. The global
inter-comparisons of PARASOL/GRASP versus MODIS showed rather robust
agreement, though some patterns and tendencies were observed. Over ocean,
PARASOL/Models and MODIS/DT AOD agree well with the correlation coefficient
of 0.92. Over land, the correlation between PARASOL/Models and the different
MODIS products is lower, ranging from 0.76 to 0.85. There is no significant
global offset; though over bright surfaces MODIS products tend to show
higher values compared to PARASOL/Models when AOD is low and smaller values
for moderate and high AODs. Seasonal AOD means suggest that PARASOL/GRASP
products show more biomass burning aerosol loading in central Africa and
dust over the Taklamakan Desert, but less AOD in the northern Sahara. It is
noticeable also that the correlation for the data over AERONET sites are
somewhat higher, suggesting that the retrieval assumptions generally work
better over AERONET sites than over the rest of the globe. One of the
potential reasons may be that MODIS retrievals, in general, rely more on
AERONET climatology than GRASP retrievals. Overall, the analysis shows that the quality of AOD retrieval from
multi-angular polarimetric observations like POLDER is at least comparable
to that of single-viewing MODIS-like imagers. At the same time, the
multi-angular polarimetric observations provide more information on other
aerosol properties (e.g., spectral AODF, AODC, AE), as well as additional
parameters such as AAOD and SSA.
Journal Article
Direct Radiative Effects of Aerosols on Numerical Weather Forecasts—A Comparison of Two Aerosol Datasets in the NCEP GFS
by
Cheng, Anning
,
Yang, Fanglin
in
Aerosol effects
,
Aerosol optical depth
,
Aerosol optical properties
2023
This study compares aerosol direct radiative effects on numerical weather forecasts made by the NCEP Global Forecast System (GFS) with two different aerosol datasets, the Optical Properties of Aerosols and Clouds (OPAC) and MERRA-2 aerosol climatologies. The underestimation of aerosol optical depth (AOD) by OPAC over northwest Africa, central to East Africa, the Arabian Peninsula, Southeast Asia, and the Indo-Gangetic Plain, and overestimation in the storm-track regions in both hemispheres are reduced by MERRA-2. Surface downward shortwave (SW) and longwave (LW) fluxes and the top-of-the-atmosphere SW and outgoing LW fluxes from model forecasts are compared with CERES satellite observations. Forecasts made with OPAC aerosols have large radiative flux biases, especially in northwest Africa and the storm-track regions. These biases are also reduced in the forecasts made with MERRA-2 aerosols. The improvements from MERRA-2 are most noticeable in the surface downward SW fluxes. GFS medium-range weather forecasts made with the MERRA-2 aerosols demonstrated slightly improved forecast accuracy of sea level pressure and precipitation over the Indian and East Asian summer monsoon region. A stronger Africa easterly jet is produced, associated with a low pressure over the east Atlantic Ocean and west of northwest Africa. Impacts on large-scale skill scores such as 500-hPa geopotential height anomaly correlation are generally positive in the Northern Hemisphere and the Pacific and North American regions in both the winter and summer seasons.
Journal Article
Intercomparison of biomass burning aerosol optical properties from in situ and remote-sensing instruments in ORACLES-2016
by
Segal-Rozenhaimer, Michal
,
Flynn, Connor
,
Liu, Xu
in
Absorption
,
Aerosol absorption
,
Aerosol effects
2019
The total effect of aerosols, both directly and on cloud properties, remains the biggest source of uncertainty in anthropogenic radiative forcing on the climate. Correct characterization of intensive aerosol optical properties, particularly in conditions where absorbing aerosol is present, is a crucial factor in quantifying these effects. The southeast Atlantic Ocean (SEA), with seasonal biomass burning smoke plumes overlying and mixing with a persistent stratocumulus cloud deck, offers an excellent natural laboratory to make the observations necessary to understand the complexities of aerosol–cloud–radiation interactions. The first field deployment of the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign was conducted in September of 2016 out of Walvis Bay, Namibia. Data collected during ORACLES-2016 are used to derive aerosol properties from an unprecedented number of simultaneous measurement techniques over this region. Here, we present results from six of the eight independent instruments or instrument combinations, all applied to measure or retrieve aerosol absorption and single-scattering albedo. Most but not all of the biomass burning aerosol was located in the free troposphere, in relative humidities typically ranging up to 60 %. We present the single-scattering albedo (SSA), absorbing and total aerosol optical depth (AAOD and AOD), and absorption, scattering, and extinction Ångström exponents (AAE, SAE, and EAE, respectively) for specific case studies looking at near-coincident and near-colocated measurements from multiple instruments, and SSAs for the broader campaign average over the month-long deployment. For the case studies, we find that SSA agrees within the measurement uncertainties between multiple instruments, though, over all cases, there is no strong correlation between values reported by one instrument and another. We also find that agreement between the instruments is more robust at higher aerosol loading (AOD400>0.4). The campaign-wide average and range shows differences in the values measured by each instrument. We find the ORACLES-2016 campaign-average SSA at 500 nm (SSA500) to be between 0.85 and 0.88, depending on the instrument considered (4STAR, AirMSPI, or in situ measurements), with the interquartile ranges for all instruments between 0.83 and 0.89. This is consistent with previous September values reported over the region (between 0.84 and 0.90 for SSA at 550nm). The results suggest that the differences observed in the campaign-average values may be dominated by instrument-specific spatial sampling differences and the natural physical variability in aerosol conditions over the SEA, rather than fundamental methodological differences.
Journal Article
Aerosol characteristics at the three poles of the Earth as characterized by Cloud–Aerosol Lidar and Infrared Pathfinder Satellite Observations
by
Fan, Hao
,
Zhao, Chuanfeng
,
Yang, Yikun
in
Accuracy
,
Aerosol optical depth
,
Aerosol optical properties
2021
To better understand the aerosol properties over the Arctic, Antarctic and Tibetan Plateau (TP), the aerosol optical properties were investigated
using 13 years of CALIPSO (Cloud–Aerosol Lidar and Infrared Pathfinder Satellite Observations) L3 data, and the back trajectories for air masses were also simulated using the Hybrid Single-Particle Lagrangian Integrated
Trajectory (HYSPLIT) model. The results show that the aerosol optical depth (AOD) has obvious spatial- and seasonal-variation characteristics, and
the aerosol loading over Eurasia, Ross Sea and South Asia is relatively large. The annual-average AODs over the Arctic, Antarctic and TP are
0.046, 0.024 and 0.098, respectively. Seasonally, the AOD values are larger from late autumn to early spring in the Arctic, in winter and spring in
the Antarctic, and in spring and summer over the TP. There are no significant temporal trends of AOD anomalies in the three study regions. Clean
marine and dust-related aerosols are the dominant types over ocean and land, respectively, in both the Arctic and Antarctic, while dust-related
aerosol types have greater occurrence frequency (OF) over the TP. The OF of dust-related and elevated smoke is large for a broad range of heights,
indicating that they are likely transported aerosols, while other types of aerosols mainly occurred at heights below 2 km in the Antarctic
and Arctic. The maximum OF of dust-related aerosols mainly occurs at 6 km altitude over the TP. The analysis of back trajectories of the air
masses shows large differences among different regions and seasons. The Arctic region is more vulnerable to mid-latitude pollutants than the
Antarctic region, especially in winter and spring, while the air masses in the TP are mainly from the Iranian Plateau, Tarim Basin and South Asia.
Journal Article
Stratospheric Aerosol Characteristics from the 2017–2019 Volcanic Eruptions Using the SAGE III/ISS Observations
by
Kloss, Corinna
,
Berthet, Gwenaël
,
Ratnam, Madineni Venkat
in
aerosol microphysics
,
aerosol properties
,
Aerosols
2023
In recent years (2017–2019), several moderate volcanic eruptions and wildfires have perturbed the stratospheric composition and concentration with distinct implications on radiative forcing and climate. The Stratospheric Aerosol and Gas Experiment III instruments onboard the International Space Station (SAGE III/ISS) have been providing aerosol extinction coefficient (EC) profiles at multiple wavelengths since June 2017. In this study, a method to invert the spectral stratospheric aerosol optical depth (sAOD) or EC values from SAGE III/ISS (to retrieve the number/volume size distributions and other microphysical properties) is presented, and the sensitivity of these retrievals is evaluated. It was found that the retrievals are strongly dependent on the choices of wavelengths, which in turn determine the shapes of the calculated curves. Further, we examine the changes in stratospheric aerosol spectral behavior, size distribution properties, time evolution (growth/decay) characteristics associated with subsequent moderate volcanic eruptions, namely, Ambae (15∘S, 167∘E; April and July 2018), Raikoke (48∘N, 153∘E; June 2019), and Ulawun (5∘S, 151∘E; June and August 2019), in different spatial regions. The observational period was classified with reference to Ambae eruptions into four phases (pre-Ambae, Ambae1, Ambae2, and post-Ambae). The pre-Ambae and post-Ambe periods comprise the 2017 Canadian fires and 2019 Raikoke/Ulawun eruptions, respectively. The spectral dependence of sAOD was comparable and lowest during the pre-Ambae and Ambae1 periods in all regions. The number concentration at the principal mode radius (between 0.07 and 0.2 μm) was observed to be higher during the Ambae2 period over the Northern Hemisphere (NH). The rate of change (growth/decay) in the sAOD on a global scale resembled the changes in the Southern Hemisphere (SH), unlike the time-lag-associated changes in the NH. These differences could be attributed to the prevailing horizontal and vertical dispersion mechanisms in the respective regions. Lastly, the radiative forcing estimates of Ambae and Raikoke/Ulawun eruptions, as reported in recent studies, was discussed by taking clues from other major and moderate eruptions to gain insight on their role in climate change.
Journal Article
Ambient aerosol properties in the remote atmosphere from global-scale in situ measurements
by
Katich, Joseph M.
,
Wagner, Nicholas J.
,
Schwarz, Joshua P.
in
Absorption
,
Aerosol absorption
,
Aerosol optical depth
2021
In situ measurements of aerosol microphysical, chemical,
and optical properties were made during global-scale flights from 2016–2018 as part of the Atmospheric Tomography Mission (ATom). The NASA DC-8 aircraft flew from ∼ 84∘ N to ∼ 86∘ S latitude over the Pacific, Atlantic, Arctic, and Southern oceans while
profiling nearly continuously between altitudes of ∼ 160 m and
∼ 12 km. These global circuits were made once each season.
Particle size distributions measured in the aircraft cabin at dry conditions
and with an underwing probe at ambient conditions were combined with bulk
and single-particle composition observations and measurements of water
vapor, pressure, and temperature to estimate aerosol hygroscopicity and
hygroscopic growth factors and calculate size distributions at ambient
relative humidity. These reconstructed, composition-resolved ambient size
distributions were used to estimate intensive and extensive aerosol
properties, including single-scatter albedo, the asymmetry parameter,
extinction, absorption, Ångström exponents, and aerosol optical
depth (AOD) at several wavelengths, as well as cloud
condensation nuclei (CCN) concentrations at fixed
supersaturations and lognormal fits to four modes. Dry extinction and
absorption were compared with direct in situ measurements, and AOD derived
from the extinction profiles was compared with remotely sensed AOD
measurements from the ground-based Aerosol Robotic Network (AERONET); this
comparison showed no substantial bias. The purpose of this work is to describe the methodology by which ambient
aerosol properties are estimated from the in situ measurements, provide
statistical descriptions of the aerosol characteristics of different remote
air mass types, examine the contributions to AOD from different aerosol
types in different air masses, and provide an entry point to the ATom
aerosol database. The contributions of different aerosol types (dust, sea
salt, biomass burning, etc.) to AOD generally align with expectations based
on location of the profiles relative to continental sources of aerosols,
with sea salt and aerosol water dominating the column extinction in most
remote environments and dust and biomass burning (BB) particles contributing
substantially to AOD, especially downwind of the African continent.
Contributions of dust and BB aerosols to AOD were also significant in the
free troposphere over the North Pacific. Comparisons of lognormally fitted size distribution parameters to values in
the Optical Properties of Aerosols and Clouds (OPAC) database commonly used
in global models show significant differences in the mean diameters and
standard deviations for accumulation-mode particles and coarse-mode dust. In
contrast, comparisons of lognormal parameters derived from the ATom data
with previously published shipborne measurements in the remote marine
boundary layer show general agreement. The dataset resulting from this work can be used to improve global-scale
representation of climate-relevant aerosol properties in remote air masses
through comparison with output from global models and assumptions used in
retrievals of aerosol properties from both ground-based and satellite remote sensing.
Journal Article
DeLiAn – a growing collection of depolarization ratio, lidar ratio and Ångström exponent for different aerosol types and mixtures from ground-based lidar observations
by
Wandinger, Ulla
,
Hofer, Julian
,
Ohneiser, Kevin
in
Aerosol optical properties
,
Aerosol properties
,
Aerosols
2023
This paper presents a collection of lidar-derived aerosol intensive optical properties for several aerosol types, namely the particle linear depolarization ratio, the extinction-to-backscatter ratio (lidar ratio) and the Ångström exponent. The data collection, named DeLiAn, is based on globally distributed, long-term, ground-based, multiwavelength, Raman and polarization lidar measurements, conducted mainly with lidars that have been developed at the Leibniz Institute for Tropospheric Research. The intensive optical properties are presented at two wavelengths, 355 and 532 nm, for 13 aerosol categories. The categories cover the basic aerosol types (i.e., marine, pollution, continental European background, volcanic ash, smoke, mineral dust), as well as the most frequently observed mixtures they form. This extensive collection also incorporates more peculiar aerosol categories, including dried marine aerosol that, compared to marine aerosol, exhibits a significantly enhanced depolarization ratio (up to 15 %). Besides Saharan dust, additional mineral dust types related to their source region were identified due to their lower lidar ratios (Central Asian and Middle Eastern dust). In addition, extreme wildfire events (such as in north America and Australia) emitted smoke into the stratosphere showing significantly different optical properties, i.e., high depolarization values (up to 25 %), compared to tropospheric smoke. The data collection reflects and underlines the variety of aerosol mixtures in the atmosphere and can be used for the development of aerosol-typing schemes. The paper contains the most up-to-date and comprehensive overview of optical properties from aerosol lidar measurements and, therefore, provides a solid basis for future aerosol retrievals in the frame of both spaceborne and ground-based lidars. Furthermore, DeLiAn can assist the efforts for the harmonization of satellite records of aerosol properties performed at different wavelengths.
Journal Article
Aerosol characterisation in the subtropical eastern North Atlantic region using long-term AERONET measurements
by
Cuevas, Emilio
,
Díaz, Juan P.
,
García, Rosa D.
in
Aerosol concentrations
,
Aerosol optical depth
,
Aerosol optical properties
2022
A comprehensive characterisation of atmospheric aerosols in the subtropical eastern North Atlantic has been carried out using long-term ground-based Aerosol Robotic NETwork (AERONET) photometric observations over the period 2005–2020 from a unique network made up of four stations strategically located from sea level to 3555 m on the island of Tenerife. This site can be considered a sentinel for the passage of airmasses going to Europe from Africa, and therefore the aerosol characterisation performed here adds important information for analysing their evolution during their path toward Northern Europe. Two of these stations (Santa Cruz de Tenerife – SCO – at sea level and La Laguna – LLO – at 580 m a.s.l.) are located within the marine atmospheric boundary layer (MABL), and the other two (Izaña – IZO – at 2373 m a.s.l. and Teide Peak – TPO – at 3555 m a.s.l.) are high mountain stations within the free troposphere (FT). Monthly climatology of the aerosol optical depth (AOD), Ångström exponent (AE), aerosol concentration, size distribution and aerosol optical properties has been obtained for the MABL and FT. Measurements that are quite consistent across the four sites
have been used to categorise the main atmospheric scenarios, and these measurements confirm an alternation between predominant
background conditions and predominant dust-loaded Saharan air mass conditions caused by seasonal dust transport over
the subtropical North Atlantic. Background conditions prevail in the MABL and FT for most of the year, while dust-laden conditions dominate in July and August. The MABL under background conditions appears as a well-mixed layer with a low aerosol concentration (the volume concentration, VolCon, ranges from 0.02 ± 0.01 to 0.04 ± 0.02 µm3 µm−2), a predominance of coarse-mode marine aerosols (the effective radius, Reff, changes from 1.60 ± 0.19 to 1.91 ± 0.34 µm), and a volume contribution of the fine-mode fraction Vf/Vt <0.35. The clean FT is characterised by remarkably low aerosol loading and a predominant impact of fine-mode aerosols throughout the year (Vf/Vt has a maximum value of 0.93 ± 0.13), with an average Reff of 0.16 ± 0.02 µm. However, under dust-laden conditions and mainly in summer, we observe a predominance of coarse-mode aerosols with maximum VolCon values of 0.26 ± 0.23 µm3 µm−2 for the MABL and 0.16 ± 0.12 (0.06 ± 0.05) µm3 µm−2 for IZO (TPO), and a similar and quite consistent fine-mode fraction of 0.12 ± 0.03 in the vertical within the MABL and FT. Similarities in micro-physical and optical intensive aerosol properties confirm that the Saharan Air Layer (SAL) is a well-mixed layer in terms of the particulate composition. An estimation of the difference in the aerosol loading in the 1 km layer between IZO and TPO (in terms of VolCon and AOD) is performed in this study, and this shows that aerosol loading at IZO is double that at TPO, but they have similar fine-mode fractions, effective radii and intensive optical properties. The long-term trend analysis at SCO shows a significant negative trend in the fine-mode AOD between 2005 and 2020 (−1.8 ± 0.5) × 10−5 yr−1, which might be linked to the large reduction in oil-refining SO2 emissions from the SCO refinery in 2012.
Journal Article
Black and brown carbon over central Amazonia: long-term aerosol measurements at the ATTO site
by
Pöhlker, Christopher
,
Ditas, Jeannine
,
Ming, Jing
in
Absorption
,
Absorption coefficient
,
Absorption cross sections
2018
The Amazon rainforest is a sensitive ecosystem experiencing the combined
pressures of progressing deforestation and climate change. Its atmospheric
conditions oscillate between biogenic and biomass burning (BB) dominated
states. The Amazon further represents one of the few remaining continental
places where the atmosphere approaches pristine conditions during occasional
wet season episodes. The Amazon Tall Tower Observatory (ATTO) has been
established in central Amazonia to investigate the complex interactions
between the rainforest ecosystem and the atmosphere. Physical and chemical
aerosol properties have been analyzed continuously since 2012. This paper
provides an in-depth analysis of the aerosol's optical properties at ATTO
based on data from 2012 to 2017. The following key results have been
obtained.
The aerosol scattering and absorption coefficients at 637 nm,
σsp,637 and σap,637, show a pronounced
seasonality with lowest values in the clean wet season (mean ± SD:
σsp,637=7.5±9.3 M m−1; σap,637=0.68±0.91 M m−1) and highest values in the BB-polluted dry season
(σsp,637=33±25 M m−1; σap,637=4.0±2.2 M m−1). The single scattering albedo at 637 nm,
ω0, is lowest during the dry season (ω0=0.87±0.03) and
highest during the wet season (ω0=0.93±0.04). The retrieved BC mass absorption cross sections, αabs, are
substantially higher than values widely used in the literature (i.e.,
6.6 m2 g−1 at 637 nm wavelength), likely related to thick organic
or inorganic coatings on the BC cores. Wet season values of
αabs=11.4±1.2 m2 g−1 (637 nm) and dry season
values of αabs=12.3±1.3 m2 g−1 (637 nm) were
obtained. The BB aerosol during the dry season is a mixture of rather fresh smoke from
local fires, somewhat aged smoke from regional fires, and strongly aged smoke
from African fires. The African influence appears to be substantial, with its
maximum from August to October. The interplay of African vs. South American
BB emissions determines the aerosol optical properties (e.g., the fractions
of black vs. brown carbon, BC vs. BrC). By analyzing the diel cycles, it was found that particles from elevated
aerosol-rich layers are mixed down to the canopy level in the early morning
and particle number concentrations decrease towards the end of the day. Brown
carbon absorption at 370 nm, σap,BrC,370, was found to
decrease earlier in the day, likely due to photo-oxidative processes. BC-to-CO enhancement ratios, ERBC, reflect the variability of burnt
fuels, combustion phases, and atmospheric removal processes. A wide range of
ERBC between 4 and 15 ng m−3 ppb−1 was observed with
higher values during the dry season, corresponding to the lowest ω0
levels (0.86–0.93). The influence of the 2009/2010 and 2015/2016 El Niño periods and the
associated increased fire activity on aerosol optical properties was analyzed
by means of 9-year σsp and σap time series
(combination of ATTO and ZF2 data). Significant El Niño-related
enhancements were observed: in the dry season, σsp,637
increased from 24±18 to 48±33 M m−1 and σap,
637 from 3.8±2.8 to 5.3±2.5 M m−1. The absorption Ångström exponent, åabs,
representing the aerosol absorption wavelength dependence, was mostly
<1.0 with episodic increases upon smoke advection. A
parameterization of åabs as a function of the BC-to-OA
mass ratio for Amazonian aerosol ambient measurements is presented. The brown
carbon (BrC) contribution to σap at 370 nm was obtained by
calculating the theoretical BC åabs, resulting in BrC
contributions of 17 %–29 % (25th and 75th percentiles) to
σap 370 for the entire measurement period. The BrC
contribution increased to 27 %–47 % during fire events under El
Niño-related drought conditions from September to November
2015. The results presented here may serve as a basis to understand Amazonian
atmospheric aerosols in terms of their interactions with solar radiation and
the physical and chemical-aging processes that they undergo during transport.
Additionally, the analyzed aerosol properties during the last two El Niño
periods in 2009/2010 and 2015/2016 offer insights that could help to assess
the climate change-related potential for forest-dieback feedbacks under
warmer and drier conditions.
Journal Article