Atmospheric Environment 244 (2021) 117882

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Atmospheric Environment
journal homepage: http://www.elsevier.com/locate/atmosenv

Simulation of long-term direct aerosol radiative forcing over the arctic

within the framework of the iAREA project
K.M. Markowicz a, *, J. Lisok a, P. Xian b
a
Institute of Geophysics, Faculty of Physics, University of Warsaw, Warsaw, 02-093, Poland
b
Naval Research Laboratory, Marine Meteorology Division, Monterey, USA

H I G H L I G H T S

• Anthropogenic, biogenic, and sea salt particles are the most important aerosols in the Arctic.
• The total aerosol radiative forcing in the Arctic (>70.5oN) is − 0.4 W/m2 for all-sky conditions.
• Anthropogenic aerosol radiative forcing is almost zero for all-sky conditions.
• Clouds reduce clear-sky aerosol radiative forcing by about 40%.

A R T I C L E I N F O A B S T R A C T

Keywords: This paper presents the climatology of aerosol optical properties and radiative forcing over the Arctic obtained
Aerosol within the framework of the iAREA (impact of absorbing aerosols on radiative forcing in the European Arctic)
Absorbing aerosol project. The presented data were obtained from the Navy Aerosol Analysis and Prediction System (NAAPS) and
Radiative forcing
the Fu-Liou radiative transfer model. NAAPS was used to simulate particle concentration and aerosol optical
Aerosol optical depth
depth (AOD) at 1 ◦ × 1 ◦ spatial resolution. Direct aerosol radiative forcing (ARF) was calculated for clear-sky
Single scattering albedo
and all-sky conditions based on NAAPS reanalysis (with AOD assimilation) and satellite observations of sur­
face and cloud properties. Long-term data (2003–2015) from NAAPS show that anthropogenic and biogenic
aerosol, as well as sea salt, make the most important contribution to total AOD (35 and 30%, respectively).
However, smoke (15%) and mineral dust (20%) cannot be neglected, especially during spring and summer.
Results of numerical simulations indicate mean shortwave (SW) ARF for the whole Arctic (>70.5oN) at the
Earth’s surface to be − 4 W/m2 for clear-sky and − 1.3 W/m2 for all-sky conditions, and at top of the atmosphere
(TOA) − 1.3 W/m2 and -0.4 W/m2, respectively. TOA ARF for anthropogenic and biogenic particles is only − 0.1
W/m2 for clear-sky and almost zero for all-sky conditions. For smoke and dust particles, SW ARF is very similar
for both Earth’s surface and TOA, as well as for clear-sky and all-sky conditions. For sea salt, SW ARF is the same
at the surface and at TOA: 0.6 W/m2 for clear-sky and − 0.3 W/m2 for all-sky conditions, because of negligible
solar absorption. Cloud cover reduces surface cooling (direct clear-sky SW ARF) by a factor of 40% and shifts
TOA SW ARF towards positive values.

1. Introduction
The Arctic region is currently experiencing unprecedented climate
change. The warming rate in this region is 2–3 times the global average
(IPCC, 2018). A clear manifestation of this is the dramatic decline in the
extent of Arctic sea ice observed in recent decades (Barry, 2017; Over­
land and Wang, 2013; Comiso et al., 2008). It is uncertain what factors
drive the changes observed in Arctic surface temperatures and the extent
of sea ice (Willis et al., 2018). The warming is suggested to be forced
mainly by greenhouse gases, and additionally by absorbing aerosols
(Bond et al., 2013). However, understanding the variability of the Arctic
climate is still a challenge due to strong interactions between local and
non-local drivers and feedbacks (Struthers et al., 2011; Abbatt et al.,
2019). Previous studies used model simulations to investigate how
aerosols affect the Arctic climate through the effects of scattering and
absorption on radiation, clouds, and surface ice/snow albedo (Clarke

* Corresponding author.
E-mail address: kmark@igf.fuw.edu.pl (K.M. Markowicz).

https://doi.org/10.1016/j.atmosenv.2020.117882
Received 30 October 2018; Received in revised form 27 July 2020; Accepted 23 August 2020
Available online 28 August 2020
1352-2310/© 2020 Elsevier Ltd. All rights reserved.
K.M. Markowicz et al.
and Noone, 1985; Flanner et al., 2007; Dumont et al., 2014). Ren et al.
(2020) report the aerosol produces an Arctic surface warming of +0.297
K during 1980–2018, explaining about 20% of the observed Arctic
warming during last four decades. Quinn et al. (2008) found that
anthropogenic aerosol warms the Arctic atmosphere and cools the sur­
face in all seasons. Shindell and Faluvegi (2009) reported that changes in
aerosols from 1976 to 2007 contributed 1.09 ± 0.81 ◦ C to the observed
Arctic surface temperature increase of 1.48 ± 0.28 ◦ C. However, other
numerical simulations indicated anthropogenic aerosols yielded a
negative forcing over the Arctic. Breider et al. (2017), based on the
GEOS-Chem model and the Fu-Liou radiative transfer code, reported
shortwave (SW) aerosol radiative forcing (ARF) of − 0.19 ± 0.05 W/m2
at the top of the atmosphere (TOA), which reflects the balance between
sulphate cooling (− 0.60 W/m2) and black carbon (BC) warming (+0.44
W/m2). Surface ARF from anthropogenic particles averaged over the
Arctic during 2005–2010 was − 1.20 W/m2, which was roughly equiv­
alent to the sum of the cooling from sulphate aerosols and BC warming.
These results stand in contrast to those obtained by Quinn et al. (2008),
where the direct ARF was estimated from 0.08 W/m2 during winter and
autumn to 0.92 W/m2 in spring. The significant differences in the
simulated impact of the anthropogenic aerosols were due to BC, which
in Quinn et al. (2008) is the dominant constituent of the total ARF. The
effect of BC on the climate system, especially in the Arctic region, is
highly uncertain (Bond et al., 2013). BC aerosols in the Arctic can per­
turb the radiation balance directly, through the absorption and scat­
tering of radiation, or through the reduction of high surface albedo (Dou
and De Xiao, 2016). ARF by BC can also result from aerosol-cloud in­
teractions (Twomey, 1977) and from semi-direct effect (Koch and Genio,
2010). Sand et al. (2013) showed that increased BC forcing in the Arctic
atmosphere reduces the surface air temperature in the Arctic. This effect
is due to the combination of the weakening of the northward heat
transport, caused by a reduction in the meridional temperature gradient,
and the dimming at the surface. Moreover, model simulations indicated
that atmospheric BC forcing outside the Arctic may be more important
for Arctic climate change than the forcing in the Arctic itself (Sand et al.,
2013).
Comparison of different models (AeroCom Phase II) showed that the
impact of BC aerosols on the global radiation balance is not well con­
strained (Samset et al., 2013). Both BC burden and BC ARF were well
spread (Myhre et al., 2013). Twelve global aerosol models showed that
at least 20% of the presented uncertainty in the modelled BC direct ARF
was due to diversity in the simulated vertical profile of BC mass (Samset
et al., 2013). In addition, a significant fraction of the variability came
from high altitudes, especially in the Arctic, where BC is transported
from middle latitudes. The models might have overestimated BC con­
centrations in the Arctic free troposphere, but the vertical profile of
Arctic BC is not well known due to sparse vertical measurements (Sand
et al., 2013).
Much of the aerosol in the Arctic originates from various parts of the
Earth (Willis et al., 2018). For example, a modeling study from Bour­
geois and Bey (2011) indicates that 59% of sulphates in Arctic tropo­
sphere come from the oxidation of SO2 emitted in Siberia (19%), Europe
(18%), Asia (13%), and North America (9%), while anthropogenic BC
and biomass burning BC emitted in Siberia, Europe, Asia, and North
America contribute 29, 25, 27, and 17%, respectively, to the Arctic BC
burden. However, due to the reduction of aerosol and precursor emis­
sion in Europe, Russia, and North America in recent decades, in situ
observations in the Arctic have shown a significant decline in concen­
trations of sulphate and BC aerosols since 1980 (Gong et al., 2010;
Hirdman et al., 2010). In the observations reported by Sharma et al.
(2013), atmospheric BC at three Arctic locations showed a reduction of
40% between 1990 and 2009. However, sea salt particles are increased,
due to the reduction of the sea ice extent in the Arctic (Struthers et al.,
2011). The latest data by Breider et al. (2017) showed a decrease in the
BC mass concentration of 2–3% per year over the period 1980–2010. As
a result, according to their calculation for total anthropogenic particles,
2
Atmospheric Environment 244 (2021) 117882
between 1980 and 2010, TOA-negative ARF in the Arctic decreased from
− 0.67 ± 0.06 W/m2 to − 0.19 ± 0.05 W/m2, yielding a net TOA ARF
increase of 0.48 ± 0.06 W/m2and a net warming of 0.27 ± 0.04 K at the
Arctic surface. However, Yang et al, (2014), using a climate model with
different radiative transfer model and aerosol optical properties of
aerosols, found no significant response in the average Arctic surface
temperatures to the 1975–2005 trends in sulphates and BC.
In this study, we provide an analysis of the climatology of aerosol
optical properties and ARF in the Arctic within the framework of the
iAREA (impact of absorbing aerosols on radiative forcing in the Euro­
pean Arctic) project based on the Navy Aerosol Analysis and Prediction
System (NAAPS) reanalysis, which includes aerosol optical depth (AOD)
data assimilation. This is just to show the difference between this study
and other modeling studies based on models which did not apply AOD
assimilation. Section 2 includes the description of the model and the
databases, followed by the validation of the model and the sensitivity
analysis of the radiative transfer code’s input parameters, as well as the
long-term mean aerosol optical properties. In Section 3 we discuss their
long-term mean values for the whole Arctic spatial distribution, as well
as the annual variability for selected Arctic regions. Conclusions are
summarised in section 4.
2. Model description
ARF in the Arctic is computed based on an off-line radiative transfer
model (RTM), which was interfaced with several databases including
aerosol transport model results and satellite observations. For this pur­
pose, the 200,503 version of the Fu-Liou code (Fu and Liou, 1992, 1993),
which employs the delta 2/4 stream solver and includes six shortwave
(SW, λ < 4 μm) and 12 longwave (LW, λ ≥ 4 μm) spectral bands, was
used. The Fu-Liou code is robust and is therefore suitable for computing
ARFs on a global scale. At the same time, it has sufficiently good accu­
racy for such global applications, as indicated by the inter-comparison,
with more precise RTMs performed by Myhre et al. (2009). The Fu-Liou
RTM was interfaced with various databases of optical properties (aero­
sols, clouds, and the Earth’s surface) and meteorological data to
compute the radiation fluxes on a regular grid with a horizontal reso­
lution of 1 ◦ × 1 ◦ and 25 vertical levels, ranging from the surface to the
level of about 18 km. The datasets were defined at each grid box by
simple interpolation (in time and space) of data from databases
described below. In this study, the diurnal mean (24 h) ARF was
computed from diurnal cycles. A higher time resolution was required for
the daytime than for the night-time to ensure sufficient accuracy for the
mean diurnal ARF estimates. For this purpose, the RTM was run with a
time step of 20 min for the cases in which the sun was above the horizon,
and of 3 h during the night.
The aerosol optical properties used in the study come from the long-
term (2003–2015) aerosol reanalysis product based on the Navy Aerosol
Analysis and Prediction System (NAAPS) with AOD assimilation. The
NAAPS reanalysis product includes aerosol mass concentration and
other aerosol variables associated with it, at a spatial resolution of 1 ◦ ×
1 ◦ and a temporal resolution of 6 h (Lynch et al., 2016). This reanalysis
utilises a modified version of NAAPS with a data assimilation module,
including quality-controlled retrievals of total AOD from MODIS on the
Terra and Aqua satellites, as well as the Multi-angle Imaging Spec­
troRadiometer (MISR) on Terra (Zhang et al., 2006; Zhang et al., 2008;
Hyer et al., 2011; Shi et al., 2014). The reanalysis version of NAAPS is
driven by the meteorological fields of Navy Operational Global Analysis
and Prediction System (NOGAPS; Hogan and Rosmond, 1991). NAAPS
model uses NOGAPS analysis (00, 06, 12, and 18 UTC) with associated
3-h forecast fields. NAAPS reanalysis uses the following variables:
topography, sea ice, surface stress, surface heat flux, surface moisture
flux, surface temperature, surface wetness, snow cover, stratiform pre­
cipitation, convective precipitation, lifting condensation level, cumulus
fractional coverage, cumulus cloud height, surface pressure, wind vec­
tor, temperature, and relative humidity. Parametrization of cloud and
K.M. Markowicz et al. Atmospheric Environment 244 (2021) 117882

planetary boundary layer processes in the NOGAPS model was previ­ factor (GF)
ously described by Teixeira and Hogan (2002). ( )− γi
1 − RH
NAAPS characterises anthropogenic and biogenic fine (ABF, GFi (RH) = (1)
1 − RHo
including sulphate, primary and secondary organic aerosols) aerosols,
dust, smoke, and sea salt aerosols. Physical processes related to sea salt
where RH and RHo are the ambient and reference (30%) relative hu­
particles for the NAAPS model were developed by Witek et al. (2007a).
midity, respectively. An empirical factor (γi) describes the humidity
The emission source function is based on wind speed at 10 m a.s.l. ac­
effect for each aerosol category. Parameter γi is defined as 0.5 for ABF
cording to Monahan’s formulation (Monahan et al., 1986). Similarly, a
particles, assuming 40% sulphate and 60% organic aerosols (Lynch
dust emission is driven by surface wind speed whenever the friction
et al., 2016), while γi is 0.63 for sulphate (Hänel, 1976), 0.18 for smoke
velocity exceeds a threshold value (6 m/s) and the surface moisture is
(Reid et al., 2005b), 0.46 for sea salt (Hegg et al., 2002; Ming and
under a critical value (Westphal et al., 1988). In addition, to estimate the
Russell, 2001), and zero for dust (Li-Jones et al., 1998). In addition, we
source function the surface erodible fraction value is used for each
assumed that the absorption coefficient is not affected by humidity.
model grid box. Emission of the biomass burning smoke in NAAPS
For the surface optical properties, the cloud-screened and quality-
reanalysis uses the FLAMBE database (Fire Locating and Modeling of
assured variables were derived from daily MODIS products of the sixth
Burning Emissions; Reid et al., 2009). To avoid changes in the geosta­
collection – M × D09CMG (Terra and Aqua). We defined the monthly
tionary constellation, which can be a challenge for time-consistency of
mean surface albedo at six bands: 0.459–0.479, 0.545–0.565, 0.62–0.67,
the smoke source function, the polar-orbiting version of FLABME was
0.841–0.876, 1.23–1.25, 1.628–1.652, and 2.105–2.155 μm. Their
used. In this case, MODIS-only fire products and emissions are applied
values were interpolated to the Fu-Liou spectral bands. The solar zenith
(Lynch et al., 2016). ABF includes sulphate, primary and secondary
angle variability was described by Markowicz and Witek (2011).
organic aerosols. Emissions for sulphate and its gaseous precursor SO2
Optical properties of clouds were used to compute all-sky radiative
are based on the Monitoring Atmospheric Composition & Climate/Ci­
fluxes. We assumed that the optical properties of clouds are horizontally
tyZen EU projects (MACCity) inventory 2005–2010 average (Granier
uniform. Monthly data of cloud properties were obtained from the sixth
et al., 2011; Diehl et al., 2012). SO2 converted from Dimethylsulphide
collection MODIS global product M × D08_M3, which uses the data from
(DMS), is derived from the monthly mean DMS seawater concentrations
Terra and Aqua satellites (Platnick et al., 2003). The dataset consisted of
from Lana et al. (2011), with the parameterization of emission fluxes at
cloud fraction, cloud optical thickness, temperature, height, and pres­
the air-sea interface from Saltzman et al. (1993). Primary organic
sure of the cloud top. The algorithm to obtain the monthly setup of
aerosol (POA) emission in NAAPS includes the major volatile organic
cloud-related variables for the Fu-Liou code was based on Markowicz
carbon (VOC) species that act as precursors for SOA (Secondary Organic
and Witek (2011), which allowed us to estimate the cloud fraction with
Aerosol). For this purpose the 2005–2010 monthly mean MACCity
randomly-overlapping altitude layers of clouds from satellite-derived
database for anthropogenic (industrial and transport) emissions of POA
cloud fraction of non-overlapping altitude layers.
and SOA precursors (Granier et al., 2011; Bond et al., 2004), as well as
The RTM requires information about vertical profiles of temperature,
biofuel data, are used. A detailed description of aerosol emissions, as
pressure, humidity, and ozone. Solar fluxes are strongly sensitive to
well as removal processes in NAAPS reanalysis, was presented by Lynch
water vapour content, so we used NOGAPS data (temperature, pressure,
et al. (2016).
and specific humidity) every 6 h to define these profiles. Because ozone
Aerosol optical properties in NAAPS are obtained from profiles of
concentration is not very responsive to SW and LW radiation fluxes, we
aerosol concentrations of four externally mixed aerosol species with no
used ozone vertical profiles from three-dimensional climatology –
interaction allowed. Profiles of the aerosol extinction coefficient, single
UGAMP (Li et al.,1995). The profiles were scaled to the total ozone
scattering albedo, and asymmetry parameter were obtained using bulk
content from MODIS M × D09CMG product.
values of optical properties that were derived from theory and obser­
vations. The predefined values of mass extinction, scattering efficiency,
and asymmetry parameter for four aerosol types were taken from the 2.1. NAAPS validation in the Arctic region
Optical Properties of Aerosol and Clouds (OPAC) database (Hess et al.,
1998). Such bulk parameters were defined for both SW and LW. The NAAPS AOD reanalysis was shown to validate well with the
Absorbing and extinction coefficients for ABF are weighted by more AErosol RObotic NETwork (AERONET) observations in general globally
absorbing aerosol particles generated by developing countries nowadays and regionally (Lynch et al., 2016). However, specific validation over
dominating global aerosol emission (Dubovik et al., 2002). Also, optical the Arctic region was not available. So we first present the validation
properties of smoke are treated similarly to ABF, according to Reid et al. results of NAAPS reanalysis for the Arctic region here. A few AERONET
(2005a, 2005b). A summary of the optical properties at 550 nm for sites with relatively long data records were selected for this purpose.
different species is available in Table 1 of Lynch et al. (2016). The effect They are Hornsund and Ny-Ålesund in Svalbard, Andenes in Northern
of humidity on the aerosol scattering coefficient at each model level is Scandinavia, Ittoqqortoormiit in Eastern Greenland, Resolute Bay in the
defined based on the Hänel (1976) equation of the hygroscopic growth Canadian Arctic, and Barrow in Alaska (Fig. 1). Table 1 shows the square
of correlation coefficient (R2), the root mean square error (RMSE), and

Table 1
Determination coefficient (R2), root mean square difference (RMSE), number of observation (N), bias between 550 nm AOD from NAAPS and from the ground-based
observations made by SP1a (Ny-Ålesund) and CIMEL (rest of the stations) sun photometers. In the case of the AERONET data, the lev. 2.0, ver. 2 product was used.
Measured AOD at 500 nm was convert to 550 nm based on 440/870 AE and next averaged to the NAAPS output (00, 06, 12, and 18 UTC) and to monthly mean values.
Last column shows long-term mean AOD (500 nm) obtained from AERONET observations.
Stations 6 h data Long-term monthly mean AERONET 550 nm AOD
2 2
N R RMSE Bias N R RMSE Bias

Hornsund (2005–2015) 1340 0.63 0.037 0.002 66 0.90 0.014 0.012 0.081
Ny-Ålesund (2003–2011) 896 0.49 0.033 0.010 49 0.93 0.021 0.019 0.067
Andenes (2003–2014) 1078 0.42 0.039 0.005 43 0.48 0.027 0.024 0.084
Ittoqqortoormiit (2010–2015) 1336 0.40 0.042 0.024 39 0.64 0.033 0.032 0.054
Resolute Bay (2004–2015) 1310 0.64 0.053 0.017 44 0.66 0.019 0.010 0.076
Barrow (2003–2015) 1344 0.51 0.067 0.008 66 0.73 0.021 0.017 0.088

3
K.M. Markowicz et al.
the bias between NAAPS and AERONET AOD (at 550 nm) every 6 h (if
observations were available) and for monthly means. Monthly means
AERONET AOD were calculated from daily averaged values while for
NAAPS data we used whole data set including days when AERONET
observation were not available. In the case of the 6-h data, the corre­
lation coefficient (R2) varies between 0.4 and 0.63 among the sites, and
RMSE varies between 0.033 and 0.067. Overall, the absolute value of the
mean bias is small, greater than 0.01 only for the Greenland and Reso­
lute Bay stations. Relative bias ([NAAPS-AERONET]/AERONET)
changes between 3% and 22% for 5 stations. Only for Greenland site is
about 44%. For the monthly mean data R2 is significantly higher
(0.48–0.93) and the RMSE smaller than the 6-h data, with the exception
of the Andenes site. For other stations, RMSE changes between 0.01 and
0.03. The values of the mean bias are small and positive. For the
Greenland and Andenes stations, the AOD from NAAPS is overestimated
by about 0.02–0.03 which corresponds to relative bias of 58% and 29%,
respectively (see Fig. 2).
Validation of NAAPS for fine (anthropogenic and biogenic fine plus
biomass burning smoke) and coarse (mineral dust plus sea salt) AOD has
been done with AERONET data. For this purpose the data obtained from
Spectral De-Convolution Algorithm (SDA) were used at 550 nm (see
Table S1 in the supplementary material). Data analysis includes results
from ten high latitude AERONET stations (Hornsund, Thule, Kanger­
lussuaq, Ittoqqortoormiit, Andenes Resolute Bay, Barrow, Bonanza
Creek, Tiksim Yakutsk) between 2003 and 2013. Fine-mode fraction
(fine to total AOD ratio) of NAAPS AOD, on average, is similar to that of
AERONET (65% vs. 62%). Deviation of fine-mode fraction is less than
3% for most sites, except the two sites over Siberia (6–7% higher) and
Bonanza Creen (Alaska; 8% higher). The NAAPS bias of coarse-mode
AOD is much smaller (0.001) compared to the bias of fine-mode AOD
(0.009). However, correlations for coarse AOD are low, suggesting the
model have difficulty producing the timing of coarse particle events
(Xian et al., 2019). In addition, fine-mode AOD from AERONET exhibits
great temporal variability on day-to-week time-scales. NAAPS model has
difficulty in capturing this large variability in fine-mode AOD. For some
stations NAAPS tends to overestimate in clean conditions and underes­
timate in highly polluted conditions. In previous research Sessions et al.
(2015), and Xian et al. (2019) report that it is very common for global
aerosol models.
Fig. 1. Location of the AERONET stations used for NAAPS AOD validation.
4
Atmospheric Environment 244 (2021) 117882
Validation of NAAPS AOD components (anthropogenic and biogenic
fine, biomass burning smoke, mineral dust, sea salt) is default due to fact
that decomposition of measured total AOD is not straightforward.
Therefore it can be done during events (e.g. biomass burning or mineral
dust) or based on the ship measurement (sea salt). On another hand
model can be validated with chemical data obtained from ground-based
measurements. Witek et al. (2007b) reports good agreement of NAAPS
surface sea salt concentration with shipboard measurements. For
example the correlation coefficient varied from 0.55 to 0.84 for different
experiments. On average, model overestimating the observation by
about 58%. It can be explained by high uncertainties of emission source
function. According to Jaeglé et al. (2011) and Lewis and Schwartz
(2004), sea salt is one of the most poorly constrained aerosols. Witek
et al. (2016) run NAAPS model with implemented different sea salt
emission source functions. The annual mean global sea salt AOD varies
in a large range from 0.028 to 0.112. After validation to satellite data
authors recommend the Sofiev et al. (2011) SSA emission function with
the Jaeglé et al. (2011) SST scaling factor as the best choice for global
and regional simulations of SSA. For this parametrization the global over
ocean average sea salt AOD is 0.085 while for Monahan’s source func­
tion used in this study the global mean is about 0.047 (Witek et al.,
2011) which corresponds to about 0.062 over the ocean.
Validation of NAAPS SSA (or absorption AOD) and asymmetry
parameter (or scattering phase function) is limited to completely clear-
sky conditions. In addition, AERONET recommendation for using ab­
sorption data (Level 2.0) is defined by a AOD (440 nm) threshold of 0.4.
For lower AOD the uncertainty of SSA is very high (Dubovik and King,
2000). Therefore such limitations prevent validation of NAAPS optical
properties at high latitudes.
2.2. Sensitivity study of ARF with respect to input parameter uncertainty
In this section, the sensitivity study of both SW and LW ARFs with
respect to the uncertainty of aerosol optical parameters, cloud proper­
ties, and surface albedo is discussed. In Table 2, we present the mean
value of the input parameters, which are used as a reference for the
sensitivity simulations. The calculations were run for a single location in
two cases: one for the reference values and the second for perturbations.
The perturbations are 0.02 (22% of the regional climatological mean)
for AOD, 0.02 (2%) for SSA (which corresponds to 47% for absorbing
AOD), 0.05 (8%) for asymmetry parameter, 0.2 (27%) for AE, 0.05 (7%)
for cloud fraction, 3.6 (87%) for cloud optical depth, 0.05 (9%) for
surface albedo, and 1 km for vertical distribution of aerosol extinction.
These are reasonable perturbations based on available observations. For
AOD the perturbation is equal to mean bias between NAAPS and AER­
ONET observation. For SSA and asymmetry parameter model validation
is not available for Arctic conditions because photometer retrieval is
very uncertain at low AOD (Dubovik et al., 2002). Number of available
data from Level 2.0 for Arctic stations does not allow statistical analysis.
Therefore in this case we assumed does not allow statistical analysis
based on mean spatial standard deviation. Also for contribution of un­
certainty of cloud optical depth to ARF we used mean standard devia­
tion. For these simulations, we assumed that the vertical profiles of
aerosol extinction coefficient have a Gaussian distribution. Due to the
large variability of surface albedo, we also performed simulations for the
surface albedo of 0.2 and 0.8. Tables 3 and 4 present differences in ARF
due to perturbation input parameters as well as the reference ARF (last
line) for the surface albedos of 0.2 and 0.8, respectively. In addition,
ARF sensitivity to non-spherical particles is simulated. For this purpose,
the optical properties of randomly oriented spheroid particles are used
from Optical Properties of Aerosols and Clouds (OPAC) ver. 4.0 (Koepke
et al., 2015), as well as optical properties of spherical dust aerosol from
OPAC ver. 3.1 (Hess et al., 1998). Total ARF uncertainty (δARF) is
computed from individual uncertainty (δARFi) defined by perturbations
described in Table 2
K.M. Markowicz et al.
Fig. 2. Comparison of annual cycle of 550 nm AOD obtained from ground-based observation (red bars) and NAAPS re-analysis (blue bars) for six Artic stations
(Hornsund, Ny-Ålesund, Andenes, Ittoqqortoormiit, Resolute Bay, and Barrow).
√∑
̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅
δARF = δARF 2i (2)
i of a non-spherical particle is rather low, as the difference between
For the SW ARF, the most important parameter is AOD, both for
clear- and all-sky conditions. An uncertainty in AOD of about 20%
produces almost the same error in SW ARF over dark (0.2) and bright
(0.8) surface albedo (Tables 3 and 4). The SSA and asymmetry param­
eters contribute to about 8–10% of ARF uncertainty, while AE only
contributes to 2–3%. In the case of surface albedo, the uncertainty of
0.05 leads to an ARF error of 7–14% for darker surface and about
20–30% for brighter. The effect is very small (below 1%) regarding
aerosol altitude uncertainty. The impact of cloud uncertainty for all-sky
SW ARF is about 7–8% for cloud fraction perturbation of ±0.05 and
10–11% for cloud optical depth of ±3.6. Uncertainty related to mineral
dust shape is about 6–8% for surface and TOA clear-sky and all-sky SW
5
Atmospheric Environment 244 (2021) 117882
ARF. Slightly lower values (5–6%) are obtained for LW ARF. The effect
spherical and spheroid particle extinction coefficients, single-scattering
albedos, and asymmetry parameters is small (Koepke et al., 2015; Fu
et al., 2009). However, Kok et al. (2017) reports that the common
simplification to treat dust as a spherical particle leads to underesti­
mation of extinction efficiency by 20–60% for coarse aerosols Conse­
quently, dust direct radiative forcing would be more positive than
estimated by earlier studies and likewise this study according to his
theory. For clear-sky conditions, total SW ARF uncertainty is about 26%
and 29% at the Earth’s surface and at TOA, respectively. In the case of
all-sky conditions, the uncertainty increases to 29–38%. With a much
brighter surface, TOA ARF uncertainty is very high and reaches 86% and
63% for clear- and all-sky conditions, respectively (Table 4). For the LW
K.M. Markowicz et al. Atmospheric Environment 244 (2021) 117882

Table 2 where it is close to 80%. Unlike the SW ARF, which is very sensitive to
Annual mean aerosol optical depth (AOD), single-scattering albedo (SSA), surface albedo, the LW ARF is not sensitive to surface albedo.
asymmetry parameter (g), Ångström Exponent (AE), total cloud fraction, total
cloud optical depth (COD) at 550 nm, surface albedo (ALB), altitude of
maximum aerosol extinction profile (ALT), and dust non-spherical particles 2.3. Long-term mean of optical input parameters
(SPHEROID) used to estimate the ARF uncertainties.
Parameter Mean value Perturbation Relative Clear-sky diurnal direct SW ARF is a function of aerosol optical
perturbation properties, surface albedo and incoming solar radiation at TOA. LW ARF
AOD – aerosol optical 0.092 0.02 0.22
also depends slightly on the profiles of aerosol, total water vapour
depth at 550 nm content, ozone, and temperature. Fig. 3 shows long-term (2003–2015)
SSA – single scattering 0.951 0.02 0.02 annual mean AOD at 550 nm for anthropogenic and biogenic particles,
albedo at 550 nm mineral dust, biomass-burning smoke, sea salt particles, as well as total
g – asymmetry parameter 0.644 0.05 0.08
AOD obtained from NAAPS. The anthropogenic and biogenic component
at 550 nn
AE – Ångström exponent 0.75 0.2 0.27 varies from 0.016 over Greenland to 0.067 over Northern Eurasia. The
450/1000 nm variability over the Central Arctic (area around the N pole), the Barents
Cfrac - total cloud fraction 0.682 0.05 0.07 Sea, and the Greenland Sea is rather small. For the mineral dust AOD the
COD – total cloud optical 4.14 3.6 0.87 variability in the whole domain is smaller (0.011–0.028) due to the long
depth
ALB – surface albedo at 0.58 (0.2, 0.05 0.09
distance from the source areas. Smoke AOD varies from 0.007
600 nm 0.8) (Greenland) to 0.058 (Alaska). Higher values appear in places where
ALT – altitude of aerosol 1 km 1 km frequent wildfires are observed. Significantly higher values are present
extinction peak over land (North America, Asia) than over water due to the source
SPHEROID – dust non- spherical (Koepke et al.,
location. Finally, the sea salt AOD is related to the wind speed over
spherical particles particles 2015)
ocean, the ice-free area, and the distance to the ice-free ocean. There­
fore, the peak of AOD is over northern Atlantic (0.077), while the
range, the AOD and AE errors are key parameters of ARF sensitivity. minimum over Greenland for aerosol components. Similar spatial vari­
AOD and AE contribute to the uncertainty of AOD in far-infrared, which ability is shown for total AOD, which changes from 0.04 to 0.15. In all
is the most important quantity for the LW ARF. For this ARF, the un­ cases, the AOD over Greenland is a minimum, which is consistent with
certainty is about 50%, with the exception of the TOA all-sky case, the minimum long-term mean AOD over Ittoqqortoormiit among all
AERONET sites as shown in Table 2, although NAAPS has a high bias

Table 3
Annual mean absolute uncertainty of SW and LW ARF due to errors in model input parameters under clear- and all-sky conditions. Results are obtained for 69.5◦ N
latitude, flat spectral surface albedo of 0.2, and annual mean aerosol and cloud conditions (see Table 2). The penultimate row shows reference ARF, and the last row
shows its uncertainty.
Parameters Uncertainty of SW ARF [W/m2] Uncertainty of LW ARF [W/m2]

clear-sky all-sky clear-sky all-sky

SURF TOA SURF TOA SURF TOA SURF TOA

ΔAOD = 0.02 0.93 0.62 0.49 0.26 0.08 0.06 0.04 0.02
ΔSSA = 0.02 0.36 0.27 0.26 0.17 0.03 0.01 0.01 0.00
Δg = 0.05 0.42 0.43 0.21 0.21 0.04 0.04 0.02 0.01
ΔAE = 0.2 0.11 0.08 0.05 0.03 0.16 0.10 0.07 0.04
ΔALB = 0.05 0.35 0.39 0.16 0.20 0.00 0.00 0.00 0.00
ΔALT = 1 km 0.04 0.09 0.01 0.17 0.01 0.04 0.00 0.05
ΔCfrac = 0.05 0.00 0.00 0.17 0.14 0.00 0.00 0.02 0.01
ΔCOD = 3.6 0.00 0.00 0.24 0.15 0.00 0.00 0.03 0.00
SPHEROID 0.39 0.22 0.19 0.08 0.02 0.01 0.01 0.01
TOTAL 1.21 0.93 0.71 0.51 0.19 0.13 0.09 0.07
ARF [W/m2] − 4.73 − 3.23 − 2.42 − 1.35 0.38 0.26 0.17 0.09
δARF/ARF 0.26 0.29 0.29 0.38 0.49 0.50 0.51 0.77

Table 4
Same as Table 3, except for surface albedo of 0.8.
Parameters Uncertainty of SW ARF [W/m2] Uncertainty of LW ARF [W/m2]

clear-sky all-sky clear-sky all-sky

SURF TOA SURF TOA SURF TOA SURF TOA

ΔAOD = 0.02 0.19 0.23 0.12 0.23 0.08 0.06 0.04 0.02
ΔSSA = 0.02 0.12 0.76 0.12 0.57 0.03 0.01 0.01 0.00
Δg = 0.05 0.07 0.09 0.03 0.04 0.04 0.04 0.02 0.01
ΔAE = 0.2 0.02 0.01 0.01 0.01 0.16 0.10 0.07 0.04
ΔALB = 0.05 0.26 0.31 0.15 0.21 0.00 0.00 0.00 0.00
ΔALT = 1 km 0.01 0.11 0.03 0.11 0.01 0.04 0.00 0.05
ΔCfrac = 0.05 0.00 0.00 0.03 0.00 0.00 0.00 0.02 0.01
ΔCOD = 3.6 0.00 0.00 0.01 0.10 0.00 0.00 0.03 0.01
SPHEROID 0.08 0.14 0.05 0.12 0.02 0.01 0.01 0.01
TOTAL 0.36 0.88 0.24 0.68 0.19 0.13 0.09 0.07
ARF [W/m2] − 0.98 1.02 − 0.58 1.06 0.38 0.26 0.17 0.09
δARF/ARF 0.37 0.86 0.41 0.64 0.50 0.50 0.51 0.77

6
K.M. Markowicz et al. Atmospheric Environment 244 (2021) 117882

Fig. 3. Spatial distribution of annual long-term (2003–2015) mean of (a) anthropogenic and biogenic, (b) mineral dust, (c) smoke, (d) sea salt AOD, and (e) total
AOD at 550 nm obtained from the NAAPS reanalysis.

over the site. The minimum AOD over Greenland is likely a result of lack
of local aerosol sources and the high topography, which impedes
transport and diffusion of low-altitude aerosols. On the other hand, our
research stands in contrast to Sand et al. (2017)’s, where no significant
AOD minimum was found over Greenland, based on 16 climate models,
which did not have aerosol assimilations (AeroCom phase II). However,
AeroCOM model median also seems to have a minimum AOD spot there,
but with much smaller contrast to its surroundings. One of the possible
explanation could be that the climate models could not resolve the high
topography effect because of their coarse resolution (mostly very coarse

7
K.M. Markowicz et al.
resolution, e.g. 2.5 × 2.5◦ ). Except that, spatial distributions of NAAPS
AOD for different components shows similar patterns to the AeroCom
phase II model means. However, NAAPS validation shows slightly high
bias (around 0.01) for total AOD but for AeroCom the mean bias is quite
low (~-0.03) (see Fig. 4 Sand et al., 2017). The long-term mean NAAPS
AOD at 550 nm for latitudes >60.5oN is significantly higher, at 0.1, than
that reported by Sand et al. (2017) at 0.07. Also, the contribution of the
natural particles such as mineral dust and sea salt in total AOD is about
50–65% higher in NAAPS than in AeroCom II.
The spatial distribution of annual mean visible surface albedo (600
nm) and columnar SSA (550 nm) is presented in Fig. 4. In the Arctic, a
significant variability of the surface albedo due to sea ice, glaciers, and
snow cover is visible (Fig. 4a). For example, the surface albedo is below
0.1 about 500 km to the south of Svalbard, while it is approximately 0.8
about 500 km to the north. This is due to the North Atlantic currents
bringing relatively warm water from middle latitudes, allowing the sea
surface to be free from ice cover even during winter (Polyakov et al.,
2017). In the case of SSA, the annual mean values were computed from
NAAPS reanalysis (Fig. 4b). The spatial variability is related to chemical
composition (aerosol type) and relative humidity. The highest SSA
(about 0.97–0.99) over the North Atlantic, Greenland, and the Barents
Sea covers the region where the aerosol is dominated by sea salt parti­
cles. Over the Central Arctic, SSA is almost constant (0.95), indicating
moderately absorbing particles. Over northern Asia (Siberia), northern
Canada, and Alaska, the SSA is only about 0.92–0.93. These regions
show peaks of smoke AOD, which is responsible for the absorption of
solar radiation, especially during the summertime.
Fig. 5 shows mean profiles of the aerosol extinction coefficient for
selected regions in the Arctic from NAAPS for the four seasons. The ABF
peak is in the lower troposphere; however, during spring the profiles are
almost constant up to the upper troposphere. Dust particles are mostly
transported in the upper (summer) and middle troposphere. During
spring relatively high values of dust extinction coefficient are visible in
the entire troposphere. Smoke particles dominate during summer, while
the altitude for maximum extinction coefficients depends on the loca­
tion. For example, over Ny-Alesund and Barrow the peaks are at about
Fig. 4. Annual mean (a) visible (600 nm) surface albedo and (b) columnar aerosol single scattering albedo at 550 nm for the years 2015 and 2003–2015,
respectively.
8
Atmospheric Environment 244 (2021) 117882
1.5 km a.s.l., over Resolute Bay it is close to 3.5 km, while the profile at
Greenland station is almost constant up to about 4 km. In the case of sea
salt, the maximum extinction is at the surface layer. The reduction of the
extinction coefficient with altitude is high for all stations and during all
seasons as sea salt aerosol fall off the atmosphere quickly because of
their large sizes.
ARF is sensitive to the relative distribution of aerosol and cloud
layers; therefore, fraction of AOD above clouds is calculated. For this
purpose the profile of aerosol extinction as well as the satellite infor­
mation on cloud vertical distribution was used. The fraction of AOD
above cloud was calculated as an integration of extinction profile above
cloud top. Fig. 6 shows the probability distribution function for AOD
fraction above the highest clouds for the whole Arctic (red bars). The
average AOD fraction is 0.12 and the standard deviation is 0.03. Because
this parameter was estimated without information about cloud cover we
defined a more reliable quantity (mean AOD fraction above clouds) as
∑
3
τi fi
< τfrac >= i=13 (3)
∑
fi
i=1
where τI is the AOD fraction above the cloud “i”, and fi is the cloud
fraction determined at three cloud levels (low, middle, and high). As a
result, mean AOD fraction above clouds is 0.36 and the standard devi­
ation is 0.04. In up to 75% of cases this parameter lies within the range
0.3–0.4, which is consistent with the vertical profiles of aerosol extinc­
tion in the Arctic (Fig. 5).
3. Results
3.1. Mean ARF for the Arctic area
Table 5 shows the long-term annual mean of AOD, SW, LW, and net
(SW + LW) ARF at the Earth’s surface and at TOA for different types of
aerosols (anthropogenic and biogenic, mineral dust, smoke, sea salt),
total aerosol, aerosol at 5 km above the surface, and absorbing particles.
K.M. Markowicz et al. Atmospheric Environment 244 (2021) 117882

Fig. 5. Mean vertical profiles of aerosol extinction coefficient for ABF (a–d), dust (e–h), smoke (i–l), and sea salt particles (m–p) obtained from NAAPS reanalysis for
Ny-Alesund (blue lines), Barrow (red lines), Resolute Bay (green lines), and Ittoqqortoormiit (black lines). Four panels for each aerosol type correspond to winter
(December–February; a, e, i, m), spring (March–May; b, f, j, n), summer (June–August; c, g, k, o), and autumn (September–November; d, h, l, p), respectively.

9
K.M. Markowicz et al. Atmospheric Environment 244 (2021) 117882

Different values were reported by Quinn et al. (2008) at the surface

Fig. 6. Probability density function of AOD fraction above the highest cloud
(red bars) and mean AOD fraction above clouds (blue bars).
The latter category includes anthropogenic and biogenic, mineral dust,
and smoke aerosols. The data were averaged for the whole Arctic (north
of 70◦ N) under clear-sky and all-sky conditions. Total clear-sky SW ARF
at the surface is − 4 W/m2, with contributions of 30%, 30%, 26%, and
14% from anthropogenic and biogenic aerosol, mineral dust, smoke, and
sea salt particles, respectively. ARF by absorbing particles is around
− 3.4 W/m2, while including aerosol load above 5 km it exceeds − 0.9 W/
m2. For the TOA, the cooling is much weaker (− 1.3 W/m2 for total
aerosol), and the contribution of aerosol types is different from at the
Earth’s surface. And it is 26%, 17%, 15%, and 43% for anthropogenic
and biogenic aerosol, mineral dust, smoke, and sea salt, respectively.
The largest contribution to clear-sky TOA ARF is attributed to non-
absorbing sea salt particles, due to the effect of scattering.
According to Table 5, cloud presence reduces surface cooling by
55–60%. In the case of TOA, clouds shift the ARF towards positive
values. The mean SW all-sky TOA ARF for total aerosol is − 0.1 W/m2,
while for anthropogenic and biogenic aerosol it is nearly 0 W/m2, and
for mineral dust, smoke, and sea salt it is 0.2, 0.05, and − 0.3 W/m2,
respectively. A similar study was performed by Breider et al. (2017) who
obtained an anthropogenic ARF of − 1.20 ± 0.05 W/m2 at the surface
and of − 0.19 ± 0.05 W/m2 at TOA, for long-term average over
2005–2010 and latitudes north of 60oN and all-sky conditions. Our data
averaged for the same area show very similar results (− 1.05 W/m2 at
surface and − 0.19 W/m2 at TOA). A slightly lower value (− 0.12 W/m2
at TOA) was obtained by Sand et al. (2017) from AeroCom Phase II.
(− 0.46 W/m2) and at TOA (0.30 W/m2) for anthropogenic particles as a
result of BC dominance in ARF (Breider et al., 2017). The mean TOA ARF
for the Arctic is comparable with a globally averaged value (− 0.27
W/m2) reported by Myhre et al. (2013), based on the AeroCom Phase II.
We found that particles above 5 km have a significant impact on ARF.
In the case of the surface ARF, it is about 22–23% (clear- and all-sky)
while for TOA ARF it is 14% (clear-sky). An even higher impact in the
Arctic was reported by Samset et al. (2013) for BC above 5 km (72%) due
to both a high fraction of aerosol at high altitudes and a strong forcing
efficiency caused by high surface albedo. For all-sky conditions, TOA
ARF by particles existing above 5 km is 0.2 W/m2, while ARF for total
aerosol is negative (− 0.1 W/m2). It can be explained by the appearance
of BC particles above the bright clouds, which enhances the solar ab­
sorption in the atmosphere (Feng et al., 2013).
In the previous section, we found that 12% of AOD is above high
clouds and 35% of AOD is above all clouds (Fig. 6). However, bearing in
mind that vertical profiles obtained from NAAPS reanalysis were not
validated thoroughly over the Arctic, similarly to other models (e.g.
Goddard Chemistry Aerosol Radiation and Transport and the Copernicus
Atmosphere Monitoring Service model). Nevertheless, Markowicz et al.
(2017a) indicated that NAAPS reanalysis was a reliable source for pre­
dicting intensive biomass burning events in the Arctic in July 2015 and
its vertical distribution of smoke matched qualitatively well with
ground-based lidar observations. Recent observations of BC concentra­
tion onboard tethered balloons in Ny-Alesund (Ferrero et al., 2016;
Markowicz et al., 2017b) provide some statistics on vertical variability
during spring and summer. However, such information is very limited in
time and space and in vertical range, which usually reaches only 1–2 km.
So the data is not used here, but it could be used for future boundary
layer aerosol validation once there is sufficient data. Recall that NAAPS
reanalysis provides skilful AOD compared to the ground-based obser­
vations (Section 2.1). The uncertainties of SW ARF for total and
absorbing aerosol that mainly consists of smoke aerosols emitted from
boreal fires and transported to the Arctic during summertime, are ex­
pected to be low.
In the case of LW ARF, the uncertainty, due mainly to uncertainties in
the optical parameters used in the calculation, can be very high, as
indicated in the sensitivity experiments in Section 2.2. So the results of
this study should be interpreted with caution. LW ARF at the surface is
about 25% of the absolute value of SW ARF. The surface LW ARF is
higher than at TOA due to the existence of aerosol mostly in the lower
troposphere, where the temperature is close to the surface value.
Therefore, the far-infrared effect is more important at the surface than at
TOA (Markowicz et al., 2003). Net ARF, which is a sum of SW and LW, is
− 3.0 W/m2 and -0.7 W/m2 for total aerosol at the surface and at TOA
under clear-sky conditions, respectively. For all-sky conditions, the
respective values are − 1.9 and 0.3 W/m2. For anthropogenic and

Table 5
Annual mean AOD, clear-, and all-sky ARF [W/m2] for different aerosol types averaged for latitudes > 70.5◦ N.
Parameters AOD Sky conditions SW ARF [W/m2] LW ARF [W/m2] NET [W/m2]

SURF TOA SURF TOA SURF TOA

Anthropogenic 0.031 clear-sky − 1.29 − 0.36 0.49 0.43 − 0.80 0.07

all-sky − 0.79 − 0.01 0.26 0.26 − 0.53 0.25
Dust 0.017 clear-sky − 1.28 − 0.23 0.54 0.23 − 0.74 0.00
all-sky − 0.80 0.19 0.30 0.16 − 0.50 0.35
Smoke 0.013 clear-sky − 1.10 − 0.21 0.16 0.12 − 0.94 − 0.09
all-sky − 0.70 0.05 0.10 0.08 − 0.60 0.13
Sea Salt 0.026 clear-sky − 0.59 − 0.59 0.04 0.02 − 0.55 − 0.57
all-sky − 0.30 − 0.29 0.02 0.01 − 0.28 − 0.28
TOTAL 0.087 clear-sky − 4.00 − 1.34 0.99 0.61 − 3.01 − 0.73
all-sky − 2.42 − 0.09 0.54 0.39 − 1.88 0.31
Total aerosol above 5 km 0.016 clear-sky − 0.93 − 0.19 0.26 0.26 − 0.67 0.07
all-sky − 0.58 0.22 0.14 0.20 − 0.44 0.41
Absorbing 0.061 clear-sky − 3.36 − 0.63 1.15 0.73 − 2.21 0.10
all-sky − 2.10 0.29 0.62 0.47 − 1.48 0.76

10
K.M. Markowicz et al.
biogenic aerosol, however, the all-sky ARF is − 0.5 and 0.3 W/m2 at the
surface and at TOA, respectively. The strongest surface cooling and
simultaneous TOA warming occur for absorbing particles (− 1.5 and 0.8
W/m2). The effect of mineral dust at TOA is neutral (0 W/m2) for
clear-sky, and positive (0.4 W/m2) when clouds are included. Smoke
particles at the surface show a cooling effect (− 0.6 W/m2) and at TOA
are slightly warming (0.1 W/m2) for all-sky conditions. Finally, for sea
salt, all-sky ARF is the same at the surface and at TOA (− 0.3 W/m2) due
to negligible solar absorption. We found that aerosol higher than 5 km
above the surface has a significant cooling effect (− 0.4 W/m2) at the
surface, and warming (0.4 W/m2) at TOA, for all-sky conditions. For
clear-sky conditions, its effect on the radiation budget is negative at the
surface (− 0.7 W/m2) and positive at TOA (0.1 W/m2).
3.2. Spatial distribution of aerosol radiative forcing
Figs. 7 and 8 show the spatial distribution of annual mean ARFs by
total aerosol under clear- and all-sky conditions. The spatial variability
of ARFs is similar to AOD due to fact that ARF is in the first approxi­
mation linear function of AOD. Total aerosol SW ARF at the surface
varies from about − 10 W/m2 over the northern Atlantic to about − 1 W/
m2 over Greenland and Central Arctic. The peak of SW ARF corresponds
to the region with the highest AOD (maximum of sea salt particles). The
Pearson correlation coefficient between mean AOD and SW ARF is
− 0.83 and − 0.81 at the surface and at TOA, respectively. The spatial
distribution of TOA SW ARF is similar (Fig. 7b), but the values are
shifted toward positive. Over the northern Atlantic, the ARF is about − 7
W/m2, while over Greenland and Central Arctic it is about 1.5 W/m2. In
the case of LW radiation, the range of ARF is 0.4–2.2 W/m2 at surface
and 0.3–1.3 W/m2 at TOA. The smallest radiation effect was obtained
over the northern Atlantic and Greenland, and the highest over northern
Eurasia. The latter is in agreement with the occurrence of anthropogenic
and smoke aerosol.
The spatial variability of net ARF is similar to that of SW ARF because
LW ARF is relatively small (about 20–25% of SW ARF). Nevertheless, the
net ARF is shifted toward positive values, and varies from − 9 to − 0.5 W/
m2 at the surface and from − 7 to 2 W/m2 at TOA. The positive ARF at
TOA was obtained for Greenland and the Central Arctic region, due to
the high surface albedo. ARF for all-sky conditions shows significantly
smaller absolute values (Fig. 8), which agrees with attenuated properties
of clouds with respect to ARF. In the presented results this effect alters
ARF by about 40% at the surface. Although the spatial distributions of
ARF for clear and all-sky conditions are similar, there are some differ­
ences. The strongest cooling effect was found not only over the northern
Atlantic Ocean but also over Central and Eastern Siberia and Alaska
under all-sky conditions (Fig. 8a). At TOA, SW ARF varies spatially be­
tween − 2.4 and 0.6 W/m2. Over the Central Arctic region, the impact of
aerosol on the radiation budget is almost zero. If we include the effect in
the LW band, the net ARF over the Central Arctic region is nearly zero at
the surface and a little higher at TOA (0.5–1 W/m2).
Similar plots to Figs. 7–8 but for anthropogenic and biogenic aerosol
ARF are shown in Fig. 9 (clear-sky) and Fig. 10 (all-sky). The spatial
distribution is similar to the ARF obtained for all aerosols. However, the
absolute values are significantly smaller in comparison to the previously
mentioned cases. Surface SW ARF for clear-sky conditions varies from
− 3 W/m2 (part of Scandinavia and Russia, Northern Atlantic, and
Barents Sea) to nearly 0 W/m2 over Greenland and the Central Arctic
region. TOA SW ARF varies between − 1.5 W/m2 (part of Scandinavia
and Russia, Northern Atlantic, and Barents Sea) and 0.5 W/m2 (Southern
Greenland). For all-sky conditions, the SW ARF varies between − 1.5 and
0 W/m2 at the Earth’s surface and between − 0.5 and 0.5 W/m2 at TOA,
with the same regions of extreme values. The spatial variability of LW
ARF is significant only for clear-sky conditions. Simulation yields the
highest values for the northern part of Eurasia, and a very small radia­
tion impact over Greenland. TOA net ARF varies between − 1 and 0.8 W/
m2 for clear-sky conditions and between − 0.5 and 0.9 W/m2 for all-sky
11
Atmospheric Environment 244 (2021) 117882
conditions, with the highest values observed over Greenland and lowest
over Northern Atlantic Ocean. Similar spatial patterns for anthropogenic
all-sky ARF were found by Sand et al. (2017). The maximum ARF re­
ported over Greenland (up to 1 W/m2) is slightly higher than in this
study. Also, the negative ARF over northern Eurasia (up to − 1 W/m2)
obtained from AeroCom II is higher than those obtained in this study (up
to − 1.5 W/m2).
3.3. Statistics of ARF over selected regions of the Arctic
A set of demonstrative regions is chosen for further illustration of the
results the discussions below. They are “Greenland” (28◦ -55◦ W, 60◦ -
80◦ N), “Svalbard” (5◦ -30◦ E, 75◦ -83◦ N), and “Central Arctic” (85◦ -90◦ N).
These regions were selected in the European Arctic to show difference of
ARF due to surface reflectance and distance to middle latitudes. Table 6
shows annual mean AOD, SSA, and net ARF at the surface and at TOA for
clear-sky and all-sky conditions for these regions. Among the three re­
gions, the most polluted is Svalbard, with mean AOD of 0.1 at 550 nm,
and with sea salt as the most important contributor. Over Greenland,
AOD is dominated by anthropogenic and biogenic aerosols and mineral
dust, while over the Central Arctic region, the prevailing impactors are
the anthropogenic and biogenic aerosols and sea salt particles. There are
some differences in ARF between the regions. Over Greenland and the
Central Arctic region surface ARF is negative and TOA ARF is positive,
except for the case of sea salt. In Svalbard, both ARFs are negative under
clear-sky and all-sky conditions, and TOA ARF is positive for mineral
dust, the absorbing aerosol category, and aerosol above 5 km. For all-sky
conditions, anthropogenic and biogenic aerosol perturbs the net radia­
tion budget at the surface and at TOA by about − 0.3 and 0.5 W/m2 over
Greenland and the Central Arctic while by − 0.7 and 0 W/m2 F. For
absorbing aerosols, the all-sky ARFs are − 0.7 and 1.4 W/m2 for
Greenland, − 1.7 and 0.1 W/m2 for Svalbard, and − 0.8 and 1.4 W/m2 at
the surface and at TOA, respectively, for the Central Arctic region. The
effect of smoke particles in the perturbation of the radiation budget is
significant, even though the contribution of biomass burning particles to
total AOD is the smallest for each region. All-sky ARF for particles above
5 km is − 0.4 and 0.9 W/m2 in Greenland, − 0.5 and 0.2 on Svalbard, and
− 0.3 and 0.6 W/m2 in the Central Arctic region, at the surface and at
TOA, respectively. We found that the most significant differences be­
tween regions are observed at TOA ARF, where negative or positive
radiation effects rely on the surface albedo.
3.4. Annual variability of AOD and ARF for selected regions
Annual variability of monthly mean AOD and its components for
three selected regions and for the whole Arctic (>70◦ N) is shown in
Fig. 11. The time variability of total AOD (Fig. 11a) is a consequence of
the different cycles of aerosol components. For anthropogenic and
mineral dust particles (Fig. 11b and c), the peaks are observed during
spring, while for smoke (Fig. 11d), they occur in summer, and for sea salt
– during autumn and winter. The increase of AOD due to anthropogenic
aerosol in spring is a phenomenon known as the Arctic haze (Shaw,
1987; Quinn et al., 2007; Tomasi et al., 2007; Tomasi et al., 2012). It is
related to aerosol transport from middle latitudes (Willis et al., 2018).
Results of long-term (1963–2015) simulation by the Hybrid
Single-Particle Lagrangian Integrated Trajectory model (HYSPLIT; Stein
et al., 2015) (see supplement material, Fig. S1) show that global air
pollution crossroads over Svalbard. The most common source region for
144 h back-trajectories ended over Ny-Alesund at 0.5 km is Northern
Asia (Siberia). In case of the back-trajectories ended at 2, 5, and 10 km
the air mass is mostly transported from Western Europe and Atlantic
Ocean, Eastern North America and Central North America, respectively.
Relative frequency of air mass transport from latitude less than 550 N is
6, 17, 34 and 31% for back-trajectories ended at 0.5, 2, 5, and 10 km,
respectively. This data shows also that transport from middle latitudes at
all altitudes (Fig. S3) is more frequent during winter than summer.
K.M. Markowicz et al. Atmospheric Environment 244 (2021) 117882

Fig. 7. Annual mean of (a, b) SW ARF, (c, d) LW ARF, (e, f) net ARF [W/m2] for clear-sky conditions. The panels on the left-hand side (a, c, e) correspond to surface
ARF and the panels on the right-hand side (b, d, f) to TOA ARF.

12
K.M. Markowicz et al. Atmospheric Environment 244 (2021) 117882

Fig. 8. As in Fig. 7, but for all-sky conditions.

Transport from middle and low latitudes is also partially responsible 0.79). For almost every month, the anthropogenic and biogenic AOD
for the occurrence of mineral dust (Fig. 11c) in the Arctic. Therefore, the over Greenland is significantly lower in comparison to Svalbard and the
Pearson correlation coefficient between monthly mean anthropogenic Central Arctic region. The anthropogenic and biogenic aerosol contrib­
and biogenic AOD as well as mineral dust AOD is relatively high (r2 = utes about 25–40% to total AOD during springtime. The climatological

13
K.M. Markowicz et al. Atmospheric Environment 244 (2021) 117882

Fig. 9. Annual mean of anthropogenic and biogenic (a, b) SW and (c, d) LW as well as (e, f) net ARF [W/m2] for clear-sky conditions. The panels on the left-hand side
(a, c, e) correspond to the surface ARF, and the panels on the right-hand side (b, d, f) to TOA ARF.

14
K.M. Markowicz et al. Atmospheric Environment 244 (2021) 117882

Fig. 10. As in Fig. 9, but for all-sky conditions.

mean (2003–2015) smoke aerosol AOD reaches 0.03 in summer, indi­ contribution to total AOD during January and February. Over
cating a contribution of about 30–50% to total AOD. Greenland, sea salt is less important, but still contributing 40–50% to
During winter and autumn, sea salt is the dominant component, total AOD. Thus, the annual AOD cycle differs slightly between regions.
especially over Svalbard (Fig. 11e). This aerosol type has a 60–70% For example, the months for maximum AOD appearances are April and

15
K.M. Markowicz et al. Atmospheric Environment 244 (2021) 117882

Table 6
Annual mean AOD as well as clear-sky and all-sky net ARF [W/m2] for different aerosol types averaged for Greenland, Svalbard, and the Central Arctic region.
Aerosol type Sky cond. Greenland Svalbard Central Arctic Region

AOD SSA AOD SSA AOD SSA ARF [W/m2]

SURF TOA SURF TOA SURF TOA

Anth Clear 0.019 0.93 − 0.35 0.49 0.029 0.94 − 1.22 − 0.48 0.030 0.94 − 0.32 0.50
All − 0.27 0.50 − 0.70 − 0.01 − 0.26 0.47
Dust Clear 0.013 0.88 − 0.33 0.45 0.014 0.88 − 1.03 − 0.45 0.017 0.88 − 0.39 0.41
All − 0.26 0.55 − 0.61 0.13 − 0.30 0.59
Smoke Clear 0.008 0.90 − 0.32 0.30 0.010 0.91 − 0.88 − 0.33 0.012 0.91 − 0.57 0.30
All − 0.24 0.33 − 0.51 − 0.02 − 0.38 0.35
Sea Salt Clear 0.016 1.00 − 0.25 − 0.26 0.043 1.00 − 1.12 − 1.13 0.024 1.00 − 0.18 − 0.22
All − 0.15 − 0.15 − 0.52 − 0.52 − 0.10 − 0.12
TOTAL Clear 0.056 0.95 − 1.33 0.84 0.097 0.97 − 4.37 − 2.66 0.082 0.95 − 1.44 0.88
All − 0.95 1.12 − 2.38 − 0.69 − 1.02 1.17
>5 km Clear 0.023 0.93 − 0.50 0.72 0.013 0.92 − 0.82 − 0.28 0.014 0.92 − 0.39 − 0.35
All − 0.39 0.87 − 0.49 0.20 − 0.28 0.55
Absor-bing Clear 0.040 0.92 − 0.91 1.25 0.053 0.92 − 2.81 − 1.05 0.058 0.92 − 1.11 1.23
All − 0.71 1.37 − 1.66 0.13 − 0.84 1.37

Fig. 11. Monthly mean of AOD at 550 nm by (a) total aerosol, (b) anthropogenic and biogenic, (c) mineral dust, (d) smoke, and (e) sea salt obtained from NAAPS
reanalysis for all the selected regions and the whole Arctic.

16
K.M. Markowicz et al.
May for Greenland, February for Svalbard, and March and April for the
Central Arctic. NAAPS AOD annual variability shows good agreement
with ground-based observations in contrast to most of the models used
in the AeroCom II, which show a peak in AOD during summer (Sand
et al., 2017). Only a few models from AeroCom II show a late spring
maximum.
The annual cycle of clear-sky ARF is a combination of temporal
variability of diurnal TOA solar radiation (related to solar declination),
AOD, surface albedo, as well as single-scattering properties of aerosols.
Fig. 12 shows monthly mean clear-sky SW ARF at the surface in the case
of total aerosol (a), anthropogenic and biogenic aerosol (b), dust (c),
smoke (d), and sea salt (e) for the three selected regions and for the
whole Arctic. For all regions and almost all aerosol types, the maximum
radiation cooling at the surface is observed during summer, when
incoming TOA solar radiation is the highest. Only for the sea salt par­
ticles, the strongest cooling occurs during spring, because in summer sea
salt AOD is very low.
The effect of sea salt on SW ARF is significantly higher over the
Svalbard region year around, except summertime, because it is sur­
rounded by open water almost all year and it lies in a zone of high-
pressure gradient indicating enhanced production of sea salt. The total
Fig. 12. Monthly mean of (a) total, (b) anthropogenic and biogenic, (c) mineral dust, (d) smoke, and (e) sea salt clear-sky SW ARF [W/m2] at the surface for
Greenland (navy blue), Svalbard (blue), the Central Arctic region (orange), and the whole Arctic (brown).
17
Atmospheric Environment 244 (2021) 117882
SW ARF during late spring and summer is up to − 12 W/m2 over the
Svalbard region, − 8 W/m2 over the Central Arctic region, and − 5 W/m2
over Greenland. In the case of the anthropogenic and biogenic aerosols,
the monthly mean forcing is up to − 4 W/m2, -2.5 W/m2, and -1.8 W/m2
over Svalbard, the Central Arctic region, and Greenland, respectively.
The LW ARF at the surface is shown in Fig. 13. In the case of the total
aerosol, the annual cycle of the LW ARF is more closely correlated with
that of AOD than of SW ARF. Thus, the maximum effect is obtained for
spring and the minimum during autumn (Fig. 13a). Also, for the
anthropogenic and mineral dust aerosol the annual cycle is similar
(Fig. 13b). While the maximum ARF occurs during summer for smoke
(Fig. 12d), and winter for sea salt (Fig. 13e). The largest LW forcing is
obtained from dust particles, due to their absorbing characteristics in the
LW. The maximum LW ARF for mineral particles is up to 1 W/m2 during
spring. Although the uncertainty of the LW ARF is large, the annual cycle
is probably close to reality.
Finally, we discuss the all-sky TOA SW ARF. In this case, the annual
variability is different, depending on the region and aerosol type
(Fig. 14). For total aerosol, negative or zero ARF (Fig. 14a) occurs only
over Svalbard throughout the year. Over Greenland, positive forcing
appears between May and September, while for the rest of the year it is
K.M. Markowicz et al.
Fig. 13. Monthly mean of (a) total, (b) anthropogenic and biogenic, (c) mineral dust, (d) smoke, and (e) sea salt clear-sky LW ARF [W/m2] at the surface for
Greenland (navy blue), Svalbard (blue), the Central Arctic region (orange), and the whole Arctic (brown).
almost zero. For the Central Arctic region, a significant positive ARF was
computed for May, as well as negative ARF for March, and for the period
from June to September. Similar temporal variability is found for
anthropogenic and biogenic (Fig. 14b), mineral dust (Fig. 14c), and
smoke aerosol (Fig. 14d). Only sea salt ARF is negative for all regions
during the whole year, with the strongest cooling in spring and in
September (Fig. 14e). Annual variability of anthropogenic ARF reported
by Sand et al. (2017) shows also positive forcing in May for several
models and a negative peak for all models during summer (July,
August). Similar temporal variation was found for smoke, which slightly
warms the system during spring and cools it during summer. Breider
et al. (2017) showed a significant change of anthropogenic ARF in the
periods 1980–1985 and 2005–2010, with emphasis on the decline in
anthropogenic contribution to TOA ARF for spring due to the reduction
of sulphate particles at the surface (about 2–3%/year). If the trend
continues in the future, one may expect very low negative ARF or
slightly positive ARF during the Arctic haze period.
18
Atmospheric Environment 244 (2021) 117882
4. Summary and conclusions
Perturbations of the radiation budget due to aerosols over the Arctic
were discussed based on the 2003–2015 climatology of the aerosol op­
tical properties obtained from NAAPS reanalysis and radiative transfer
simulation. The most important results are the following:
- Annual AOD averaged over the Arctic (above 70.5◦ N) is 0.09 at 550
nm, while 0.09, 0.11, 0.09 and 0.06, for winter, spring, summer and
autumn, respectively.
- NAAPS AOD contribution is 34% from anthropogenic and biogenic
aerosol, 22% from mineral dust, 11% from smoke, and 33% from sea
salt. AOD shows seasonal variability with a late autumn and winter
peak for sea salt particles (53% of contribution to AOD), a spring
maximum related to the Arctic haze phenomenon dominated by
anthropogenic aerosol (40%) and sea salt (22%), and a summer peak
related to the long-range transport of smoke aerosol (34%).
- Validation of model AOD versus AERONET data shows a relatively
small bias (0.01–0.02) for most stations and a relatively good
agreement (e.g. annual variability). Only over Greenland, AOD is
K.M. Markowicz et al.
Fig. 14. Monthly mean of (a) total, (b) anthropogenic and biogenic, (c) mineral dust, (d) smoke, and (e) sea salt all-sky SW ARF [W/m2] at TOA for Greenland (navy
blue), Svalbard (blue), the Central Arctic region (orange), and the whole Arctic (brown).
significantly overestimated similarly to other models (e.g. AeroCom
phase II, Sand et al., 2012)
- Mean SW ARF for total aerosol shows strong cooling at the surface: 4
W/m2 for clear-sky and only − 1.3 W/m2 during all-sky conditions.
At TOA, ARF is also negative for both cases (− 1.3 W/m2 and -0.4 W/
m2).
- Anthropogenic and biogenic particles have a cooling influence at the
surface: 2.4 and − 0.8 W/m2 for clear-sky and all-sky conditions,
respectively. At TOA, ARF is slightly negative for clear-sky (− 0.1 W/
m2) and almost zero for all-sky conditions.
- For smoke and dust particles, the SW ARF is very similar both for the
Earth’s surface and for TOA, for clear-sky and all-sky conditions.
Only for all-sky conditions at TOA, ARF is slightly positive (0.1–0.2
W/m2).
- For sea salt, SW ARF is the same at the surface and at TOA: 0.6 W/m2
for clear-sky and − 0.3 W/m2 for all-sky conditions, as a result of
negligible solar absorption.
- Mostly due to the spatial variability of AOD and surface albedo the
mean SW ARF is sensitive to how the Arctic region is defined. If it is
considered as the region north of 60.5◦ N (expanding from 70.5oN),
19
Atmospheric Environment 244 (2021) 117882
SW ARF for anthropogenic and biogenic particles changes from
almost zero to negative values (− 0.2 W/m2) at TOA in all-sky con­
ditions. This result is similar to the value obtained during AeroCom
Phase II (Sand et al., 2017).
- Total SW ARF for the Arctic region is strongly correlated with surface
albedo. Pearson correlation coefficient between surface albedo the
surface and TOA clear-sky SW ARF is 0.92 and 0.90, respectively. For
AOD, the same quantity is 0.73, for TOA and 0.66 for surface ARF.
Negligible correlation coefficients are for SSA and surface (0.01) and
TOA (0.12) ARF.
- The annual cycle of ARF in the Arctic is mainly a function of AOD,
surface albedo, and incoming solar radiation at TOA. As a result, the
absolute value of ARF is large during both spring and summer times,
because AOD is the highest in spring and TOA solar radiation is the
maximum in summer.
- The presence of cloud covers reduces the surface cooling (direct
clear-sky SW ARF) by a factor of 40% and shifts TOA SW ARF to­
wards positive values.
- Estimated LW ARF is significantly smaller than SW ARF. For dust as
well as an anthropogenic and biogenic aerosol, LW ARF reaches 0.5
K.M. Markowicz et al.
W/m2 at the surface and 0.15–0.3 W/m2 at TOA in all-sky conditions.
Very low value (below 0.05 W/m2) has been found for sea salt TOA
and surface ARF.
- There are larger uncertainties in the LW ARF estimates than the SW
ARF estimates. The obtained values of net ARF are only an approx­
imation. A better estimation of LW ARF would require validations
and potentially better representations of aerosol size distributions
and aerosol vertical distributions in the model.
- The maximum uncertainties, by combing all maximum uncertainties
in the same direction in AFR calculation from a set of aerosol optical
properties, are between 26 and 29% for clear-sky and 29–38% for all-
sky conditions for SW AFR. While for LW ARF the numbers are 70%–
100% for clear-sky and all-sky. Very high uncertainties in LW ARF is
due to the fact that extrapolating optical properties of aerosols from
visible and infrared to far-infrared is challenging and requires vali­
dation of AOD at multiple longer wavelengths. Thus aerosol optical
properties are much better constrained for SW than for LW. Also
since satellite retrieved AOD is a column integrated variable, aerosol
speciation and vertical distribution are not constrained by assimila­
tion of AOD. The operations used to convert AOD into 3-D speciated
aerosol fields and vice versa constitute another source of uncertainty
in ARF estimation.
- A large uncertainty of ARF in the LW can be reduce by improve
model representation of aerosol size distribution in the models,
especially for coarse mode and their chemical composition. It can be
done by validation of model’s size distribution by ground-based
observation. In addition, the satellite retrieval of AOD in the
middle-infrared can help to reduce the uncertainty of far-infrared
AOD estimation
The rapid change of climate in the Arctic observed in the last de­
cades, with the increase in the surface temperature and the reduction of
the ice extent, has modified the aerosol impact on the Arctic system. The
reduction of surface albedo is moving the ARF towards negative values,
as is the increase of sea salt emission from ice-free regions (Struthers
et al., 2011). Therefore, the effect of aerosol on the Arctic amplification
will probably decrease; however, detailed research is needed.
CRediT authorship contribution statement
K.M. Markowicz: Conceptualization, Methodology, Writing - orig­
inal draft. J. Lisok: Input to model preparation, Visualization, Writing -
review & editing. P. Xian: Formal analysis, Validation, NAAPS re-
analysis preparation, model validation, Writing - review & editing.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgements
The authors would like to acknowledge the support for this research
from the Polish-Norwegian Research Programme operated by the Na­
tional Center for Research and Development under the Norwegian
Financial Mechanism 2009–2014 within the framework of the Project
Contract No. Pol-Nor/196911/38/2013. The authors also acknowledge
Brent Holben and Piotr Sobolewski for the use of the data from the
AERONET station in Hornsund, Victoria E. Cachorro Revilla and Sandra
Blindheim for the data from the Andenes AERONET station, Rick
Wagener for Ittoqqortoormiit, Ihab Abboud and Vitali Fioletov for
Resolute Bay, and for Barrow AERONET station data. The data from Ny-
Ålesund sun-photometer were provided by the Alfred Wegener Institute
for Polar and Marine Research. Dr. Xian’s Arctic NAAPS reanalysis work
was sponsored by NASA Grant NNH17AE58I on behalf of the Aura
20
Atmospheric Environment 244 (2021) 117882
Science Team and Atmospheric Composition Modeling and Analysis
Program and the U.S. Office of Naval Research code 322.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.atmosenv.2020.117882.
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