Atmospheric chemistry and physics,
Journal Year:
2023,
Volume and Issue:
23(21), P. 13911 - 13940
Published: Nov. 8, 2023
Abstract.
A
large
part
of
the
uncertainty
in
climate
projections
comes
from
uncertain
aerosol
properties
and
aerosol–cloud
interactions
as
well
difficulty
remotely
sensing
them.
The
southeastern
Atlantic
functions
a
natural
laboratory
to
study
biomass-burning
smoke
constrain
this
uncertainty.
We
address
these
gaps
by
comparing
Weather
Research
Forecasting
with
Chemistry
Community
Atmosphere
Model
(WRF-CAM5)
multi-campaign
observations
ORACLES
(ObseRvations
Aerosols
above
CLouds
their
intEractionS),
CLARIFY
(CLoud–Aerosol–Radiation
Interaction
Forcing),
LASIC
(Layered
Smoke
Interactions
Clouds)
August
2017
evaluate
range
model's
chemical
properties,
size
distributions,
processes,
transport,
interactions.
Overall,
while
WRF-CAM5
is
able
represent
some
key
discrepancies
highlight
need
for
further
analysis.
Observations
composition
show
an
overall
decrease
mean
diameter
ages
over
4–12
d,
model
lacks
trend.
mass
ratio
organic
(OA)
black
carbon
(BC),
OA:BC,
OA
monoxide
(CO)
mixing
ratio,
OA:CO,
suggests
that
missing
processes
selectively
remove
particle
phase,
such
photolysis
heterogeneous
chemistry.
(factor
∼2.5)
enhancement
sulfate
free
troposphere
(FT)
boundary
layer
(BL)
not
present
model,
pointing
importance
properly
representing
secondary
formation
marine
dimethyl
sulfide
gaseous
SO2
emissions.
shows
persistent
overprediction
aerosols
(MBL),
especially
clean
conditions,
which
multiple
pieces
evidence
link
weaker
removal
modeled
MBL
than
reality.
This
includes
several
features,
observed
shifts
towards
smaller
diameters,
inaccurate
concentration
ratios
carbon,
underprediction
heavy
rain
events,
little
biases
entrainment.
average
below-cloud
activation
fraction
(NCLD/NAER)
remains
relatively
constant
between
field
campaigns
(∼0.65),
it
decreases
substantially
(∼0.78)
(∼0.5),
could
be
due
misrepresentation
conditions.
also
overshoots
upper
limit
on
liquid
cloud
droplet
around
NCLD=
400–500
cm−3
overpredicts
spread
NCLD.
related
often
drastically
overestimating
strength
vertical
turbulence
up
factor
10.
expect
results
motivate
similar
evaluations
other
modeling
systems
promote
development
reduce
critical
uncertainties
simulations.
Atmospheric chemistry and physics,
Journal Year:
2021,
Volume and Issue:
21(22), P. 16689 - 16707
Published: Nov. 16, 2021
Abstract.
In
2016–2018,
the
ObseRvations
of
Aerosols
above
CLouds
and
their
intEractionS
(ORACLES)
project
undertook
3-month-long
deployments
to
southeastern
(SE)
Atlantic
Ocean
using
research
aircraft
better
understand
impact
biomass
burning
(BB)
aerosol
transport
SE
on
climate.
this
(part
1
meteorological
overview)
paper,
climatological
features
at
monthly
timescales
are
investigated.
The
southern
African
easterly
jet
(AEJ-S),
defined
as
zonal
easterlies
over
600–700
hPa
exceeding
6
m
s−1
around
5–15∘
S,
is
a
characteristic
feature
mid-level
circulation
Africa
that
was
also
during
deployment
months
August
2017,
September
2016,
October
2018.
Climatologically,
AEJ-S
develops
lower
altitudes
(∼
3
km;
700
hPa)
between
5–10∘
S
in
August,
while
it
4
km
600
further
south
(5–15∘
S)
October,
largely
driven
by
strong
sensible
heating
plateau.
Notable
anomalous
characteristics
months,
compared
climatology
(2000–2018),
include
following:
(1)
weaker
than
mean,
with
an
additional
upper-level
aloft
km)
10∘
S.
2017
drier
climatology,
stronger
Benguela
low-level
(LLJ)
925–950
along
Namibian
coast
Atlantic.
Consistent
this,
anticyclone
closer
mean.
(2)
During
intensity
similar
although
heat
low
vertical
motion
land
slightly
climatology.
LLJ
large-scale
were
(3)
2018,
anticyclone.
2018
wetter
coastal
region
all
sea
surface
temperatures
(SST)
warmer
means,
but
mean
cloud
fraction
only
noticeably
reduced
2017.
A
weak
can
explain
offshore
black
carbon
(BC)
mixing
ratios
within
European
Centre
for
Medium-Range
Weather
Forecasts
(ECMWF)
Copernicus
Atmosphere
Monitoring
Service
(CAMS)
reanalysis,
BC
peak
altitude,
2–3
km,
below
AEJ-S.
wave
disturbance
associated
weakening
through
reduction
strength
Abstract
Southern
Africa
produces
a
third
of
global
biomass
burning
emissions,
which
have
long
atmospheric
lifetime
and
influence
regional
radiation
balance
climate.
Here,
we
use
airmass
trajectories
to
link
different
aircraft
observations
investigate
the
evolution
biomass-burning
aerosols
during
their
westward
transport
from
over
south-eastern
Atlantic,
where
semi-permanent
stratocumulus
cloud
deck
is
located.
Our
results
show
secondary
organic
aerosol
formation
initial
3
days
transport,
followed
by
decreases
in
via
photolysis
before
reaching
equilibrium.
Aerosol
absorption
wavelength
dependency
with
ageing,
due
an
increase
particle
size
photochemical
bleaching
brown
carbon.
Cloud
processing,
including
aqueous-phase
reaction
scavenging,
contributes
oxidation
aerosols,
while
it
strongly
reduces
large
diameter
particles
single-scattering
albedo
aerosols.
Together,
these
processes
resulted
marine
boundary
layer
fewer
yet
more
oxidized
absorbing
Atmospheric chemistry and physics,
Journal Year:
2022,
Volume and Issue:
22(18), P. 12113 - 12151
Published: Sept. 19, 2022
Abstract.
Smoke
from
southern
Africa
blankets
the
southeastern
Atlantic
Ocean
June
to
October,
producing
strong
and
competing
aerosol
radiative
effects.
effects
on
transition
between
overcast
stratocumulus
scattered
cumulus
clouds
are
investigated
along
a
Lagrangian
(air-mass-following)
trajectory
in
regional
climate
large
eddy
simulation
models.
Results
compared
with
observations
three
recent
field
campaigns
that
took
place
August
2017:
ObseRvations
of
Aerosols
above
CLouds
their
intEractionS
(ORACLES),
Aerosol
Radiative
Impacts
Forcing:
Year
2017
(CLARIFY),
Layered
Interactions
Clouds
(LASIC).
The
case
study
is
set
up
around
joint
ORACLES–CLARIFY
flight
near
Ascension
Island
18
2017.
sampled
upstream
an
ORACLES
15
likely
entrained
into
marine
boundary
layer
later
during
flight.
first
simulated
WRF-CAM5
model
distinct
setups:
(1)
FireOn,
which
smoke
emissions
any
resulting
smoke–cloud–radiation
interactions
included;
(2)
FireOff,
no
(3)
RadOff,
microphysical
included
but
does
not
interact
directly
radiation.
Over
course
trajectory,
differences
free
tropospheric
thermodynamic
properties
FireOn
FireOff
nearly
identical
those
showing
aerosol–radiation
primarily
responsible
for
These
non-intuitive:
addition
expected
heating
within
core
plume,
there
also
“banding”
effect
cooler
temperature
(∼1–2
K)
greatly
enhanced
moisture
(>2
g
kg−1)
at
plume
top.
This
banding
caused
by
vertical
displacement
former
continental
troposphere
anomalous
diabatic
due
absorption
sunlight
manifests
as
few
hundred
meters
per
day
reduction
large-scale
subsidence
over
ocean.
A
(LES)
then
forced
fields
taken
outputs
runs.
Cases
run
selectively
perturbing
one
variable
(e.g.,
number
concentration,
temperature,
moisture,
velocity)
time
better
understand
contributions
different
indirect
(microphysical),
“large-scale”
semi-direct
(above-cloud
changes),
“local”
(below-cloud
absorption)
Despite
more
than
5-fold
increase
cloud
droplet
concentration
when
including
concentrations,
minimal
fraction
evolution
LES
comparing
base
perturbed
dynamic
forcings.
factor
2
decrease
background
concentrations
shifts
classical
entrainment-driven
“deepening–warming”
trade
precipitation-driven
“drizzle-depletion”
open
cells,
however.
changes
WRF-simulated
adjustments
strongly
influence
terms
both
rate
deepening
(especially
inversion
jump
subsidence)
final
effect).
Such
would
have
been
possible
simulate
using
small-domain
alone.
Atmospheric chemistry and physics,
Journal Year:
2022,
Volume and Issue:
22(4), P. 2769 - 2793
Published: March 2, 2022
Abstract.
Aerosol–cloud–precipitation
interactions
(ACIs)
provide
the
greatest
source
of
uncertainties
in
predicting
changes
Earth's
energy
budget
due
to
poor
representation
marine
stratocumulus
and
associated
ACIs
climate
models.
Using
situ
data
from
329
cloud
profiles
across
24
research
flights
NASA
ObseRvations
Aerosols
above
CLouds
their
intEractionS
(ORACLES)
field
campaign
September
2016,
August
2017,
October
2018,
it
is
shown
that
contact
between
above-cloud
biomass
burning
aerosols
over
Southeast
Atlantic
Ocean
was
with
precipitation
suppression
a
decrease
susceptibility
(So)
aerosols.
The
173
“contact”
aerosol
concentration
(Na)
greater
than
500
cm−3
within
100
m
tops
had
50
%
lower
rate
(Rp)
20
So,
on
average,
compared
156
“separated”
Na
less
up
at
least
tops.
Contact
separated
statistically
significant
differences
droplet
(Nc)
effective
radius
(Re)
(95
confidence
intervals
two-sample
t
test
are
reported).
84
90
higher
Nc
1.4
1.6
µm
Re
profiles.
In
clean
boundary
layers
(below-cloud
350
cm−3),
25
31
0.2
0.5
Re.
polluted
exceeding
98
108
1.8
On
other
hand,
insignificant
average
liquid
water
path,
thickness,
meteorological
parameters
like
surface
temperature,
tropospheric
stability,
estimated
inversion
strength.
These
results
suggest
microphysical
properties
were
driven
by
rather
effects,
adjustments
existing
relationships
Rp
model
parameterizations
should
be
considered
account
for
role
ACIs.
Atmospheric Research,
Journal Year:
2022,
Volume and Issue:
278, P. 106359 - 106359
Published: July 25, 2022
Mineral
dust
contributes
to
more
than
half
of
the
global
aerosol
loading.
However,
radiative
impacts
aerosols
on
planetary
boundary
layer
(PBL)
structure
have
not
been
explored
sufficiently.
During
a
typical
storm
event
over
Tarim
Basin,
exhibit
well-mixed
distribution
during
daytime
in
spite
shallow
particles
accumulated
at
higher
altitudes.
By
contrast,
nocturnal
plumes
are
located
near
surface
due
stable
stratification.
We
demonstrate
that
these
differentiated
vertical
distributions
determine
spatial
heterogeneity
loading,
fluxes
and
PBL
height
variations.
Dust
cause
suppression
nighttime
promotion
through
modulating
atmospheric
budgets.
Specifically,
dust-induced
cooling
effect
within
directly
inhibits
development.
is
then
amplified
by
entrainment
processes
resulting
excessively
low
height,
especially
for
below
but
top.
weaken
updrafts
from
downdrafts
free
atmosphere,
which
further
reduce
mixing
attenuating
horizontal
advection,
eventually
amplify
suppression.
At
night,
near-surface
stimulate
warm
unstable
lower
generate
advection
heating
promote
Our
study
highlights
importance
specifying
parameters
activities
quantifying
dust-PBL
interactions.
Atmospheric chemistry and physics,
Journal Year:
2022,
Volume and Issue:
22(21), P. 14209 - 14241
Published: Nov. 8, 2022
Abstract.
Part
1
(Ryoo
et
al.,
2021)
provided
a
climatological
overview
of
the
ObsErvation
Aerosols
above
CLouds
and
their
intEractionS
(ORACLES)
period
assessed
representativeness
deployment
years.
In
part
2,
more
detailed
meteorological
analyses
support
interpretation
airborne
measurements
for
aerosol
transport
its
interaction
with
low
clouds
over
southeastern
(SE)
Atlantic
Ocean
during
September
2016,
August
2017,
October
2018
deployments
at
daily
synoptic
scale.
The
key
characteristics
2016
are
(1)
southern
African
easterly
jet
(AEJ-S),
centered
around
600
hPa
(∼4
km),
which
strengthens
throughout
month
in
concert
warming
continental
heat
low,
strongest
winds
occurring
23
September.
These
advect
both
moisture
free
troposphere.
(2)
Mid-tropospheric
black
carbon
(BC)
is
entrained
times
into
boundary
layer,
(3)
convection
land
dry
south
about
10∘
S
moist
north
S.
mean
low-cloud
fraction
(low
CF)
well
correlated
high
tropospheric
stability
(LTS,
r=0.44–0.73
flight
domain;
0–10∘
E,
5–25∘
S)
moderately
layer
height
(BLH,
r=0.37–0.52),
defined
as
altitude
maximum
vertical
gradient
moisture.
For
2017
deployment,
primary
that
AEJ-S
lower
(∼3
km;
∼700
hPa)
further
(5–7∘
than
only
becomes
established
by
20
August,
separate
present
aloft
500
(∼5.5
km)
before
that,
mid-tropospheric
BC–RH
coupling
after
develops,
3
km,
CF
less
closely
LTS
(r=0.16–0.57)
BLH
(r=0.11–0.25)
(4)
reaches
700
Namibian–Kalahari
dryland
(∼15–25∘
S,
∼18–24∘
E),
generating
plume
subsequently
advected
AEJ-S.
develops
hPa,
driven
Kalahari
(∼10–25∘
∼12–24∘
but
it
diminishes
time
moves
southward,
offshore
advection
BC
water
vapor
strongly
modulated
8–10∘
early
October,
this
decreases
mid-latitude
frontal
systems
develop
weakens
mid-to-late
AEJ-S–low-level
(LLJ)
coastal
Namibian
region
relationship
among
all
months,
largely
reduced
strong
LLJ,
especially
to
cloud
deck's
south,
insignificant
compared
other
2
partially
due
variability
introduced
passage
disturbance.