Abstract.
Marine
emissions
of
dimethyl
sulfide
(DMS)
and
the
subsequent
formation
its
oxidation
products
methane
sulfonic
acid
(MSA)
sulfuric
(H2SO4)
are
well-known
natural
precursors
atmospheric
aerosols,
contributing
to
particle
mass
cloud
over
ocean
coastal
regions.
Despite
a
long-recognized
well-studied
role
in
marine
troposphere,
DMS
chemistry
remains
work
progress
within
many
current
air
quality
climate
models,
with
recent
advances
exploring
heterogeneous
uncovering
previously
unknown
intermediate
species.
With
identification
additional
pathways
species
influencing
eventual
fate,
it
is
important
understand
impact
these
on
overall
sulfate
aerosol
budget
size
distribution.
In
this
work,
we
update
evaluate
mechanism
chemical
transport
model
GEOS-Chem
by
implementing
expanded
into
model.
These
updates
include
gas-
aqueous-phase
reactions,
intermediates
sulfoxide
(DMSO)
sulphinic
(MSIA),
as
well
loss
uptake
recently
quantified
hydroperoxymethyl
thioformate
(HPMTF).
We
find
that
updated
collectively
decreases
global
mean
surface-layer
gas-phase
sulfur
dioxide
(SO2)
mixing
ratio
38
%
enhances
(SO42-)
16
%.
further
perform
sensitivity
analyses
contribution
HPMTF
budget.
Comparing
modeled
concentrations
available
observations
improved
biases
relative
previous
studies.
To
quantify
impacts
distributions
concentration
use
TOMAS
microphysics
module,
finding
changes
growth
affect
distribution
aerosol.
new
DMS-oxidation
scheme
annual
surface
layer
number
particles
diameters
smaller
than
80
nm
12
%,
processes
related
mostly
responsible
for
reduction.
However,
larger
increases
4.5
suggesting
promotes
seasonal
sizes
capable
acting
condensation
nuclei
(CCN).
Atmospheric
amines,
derivatives
of
ammonia,
play
a
unique
yet
not
fully
understood
role
in
air
quality,
climate
and
public
health.
Sub-5
parts
per
trillion
Volume
(pptV,
<10-12
volume)
mixing
ratios
amines
facilitate
the
physical
and/or
chemical
transformation
aerosols
atmosphere,
enhancing
aerosol
formation
growth
rates,
hygroscopicity,
activation
cloud
condensation
nuclei.
This
serves
as
initial
step
for
droplet
and,
consequently,
influences
properties
hydrological
cycle.
Ambient
observations
demonstrate
more
than
thousand-fold
particle
rates
presence
compared
to
ammonia.
Yet,
challenges
related
detecting
minute
levels
paucity
ambient
amine
measurements,
limited
process-based
understanding
airborne
production
have
resulted
being
underrepresented
global
models.
Therefore,
advanced
techniques
with
extremely
low
detection
limits
highly
spatially
temporally
resolved
measurements
globally
diverse
environments
are
essential.
Amines,
ubiquitous
atmospheric
compounds
that
emitted
from
range
natural
anthropogenic
sources,
key
activating
nuclei,
under-represented
models
require
future
high-precision
measurement.
Atmospheric chemistry and physics,
Journal Year:
2024,
Volume and Issue:
24(6), P. 3379 - 3403
Published: March 19, 2024
Abstract.
Marine
emissions
of
dimethyl
sulfide
(DMS)
and
the
subsequent
formation
its
oxidation
products
methanesulfonic
acid
(MSA)
sulfuric
(H2SO4)
are
well-known
natural
precursors
atmospheric
aerosols,
contributing
to
particle
mass
cloud
over
ocean
coastal
regions.
Despite
a
long-recognized
well-studied
role
in
marine
troposphere,
DMS
chemistry
remains
work
progress
within
many
current
air
quality
climate
models,
with
recent
advances
exploring
heterogeneous
uncovering
previously
unknown
intermediate
species.
With
identification
additional
pathways
species
that
influence
eventual
fate
DMS,
it
is
important
understand
impact
these
on
overall
sulfate
aerosol
budget
size
distribution.
In
this
work,
we
update
evaluate
mechanism
chemical
transport
model
GEOS-Chem
by
implementing
expanded
model.
These
updates
include
gas-
aqueous-phase
reactions,
intermediates
sulfoxide
(DMSO)
methanesulfinic
(MSIA),
loss
uptake
recently
quantified
hydroperoxymethyl
thioformate
(HPMTF).
We
find
updated
collectively
decreases
global
mean
surface-layer
gas-phase
sulfur
dioxide
(SO2)
mixing
ratio
40
%
enhances
(SO42-)
17
%.
further
perform
sensitivity
analyses
contribution
HPMTF
budget.
Comparing
modeled
concentrations
available
observations,
improved
biases
relative
previous
studies.
To
quantify
impacts
distributions
concentration,
use
TwO-Moment
Aerosol
Sectional
(TOMAS)
microphysics
module
coupled
changes
growth
affect
distribution
aerosol.
new
DMS-oxidation
scheme,
annual
number
concentration
particles
diameters
smaller
than
80
nm
16.8
%,
processes
related
being
mostly
responsible
for
reduction.
However,
larger
(corresponding
capable
acting
as
condensation
nuclei,
CCN)
increases
3.8
suggesting
scheme
promotes
seasonal
sizes.
RSC Advances,
Journal Year:
2024,
Volume and Issue:
14(19), P. 13321 - 13335
Published: Jan. 1, 2024
The
acidity
of
the
acid,
nature
nucleophilic
agents,
type
aldehyde,
proton
transferall
play
significant
roles
in
nucleation
process
aldehyde-sulfur-based
particles.
npj Climate and Atmospheric Science,
Journal Year:
2024,
Volume and Issue:
7(1)
Published: July 13, 2024
Abstract
Natural
aerosols
are
an
important,
yet
understudied,
part
of
the
Arctic
climate
system.
marine
biogenic
aerosol
components
(e.g.,
methanesulfonic
acid,
MSA)
becoming
increasingly
important
due
to
changing
environmental
conditions.
In
this
study,
we
combine
in
situ
observations
with
atmospheric
transport
modeling
and
meteorological
reanalysis
data
a
data-driven
framework
aim
(1)
identify
seasonal
cycles
source
regions
MSA,
(2)
elucidate
relationships
between
MSA
variables,
(3)
project
response
based
on
trends
extrapolated
from
variables
determine
which
contributing
these
projected
changes.
We
have
identified
main
areas
be
Atlantic
Pacific
sectors
Arctic.
Using
gradient-boosted
trees,
were
able
explain
84%
variance
find
that
most
for
indirectly
related
either
gas-
or
aqueous-phase
oxidation
dimethyl
sulfide
(DMS):
shortwave
longwave
downwelling
radiation,
temperature,
low
cloud
cover.
undergo
shift,
non-monotonic
decreases
April/May
increases
June-September,
over
next
50
years.
Different
different
months
driving
changes,
highlighting
complexity
influences
natural
component.
Although
oceanic
(sea
surface
DMS
emissions,
sea
ice)
precipitation
remains
seen,
here
show
will
likely
shift
solely
changes
variables.
Environmental Science & Technology,
Journal Year:
2023,
Volume and Issue:
57(34), P. 12741 - 12751
Published: Aug. 14, 2023
Marine
biological
activities
make
a
non-negligible
contribution
to
atmospheric
aerosols,
leading
potential
impacts
on
the
regional
environment
and
climate.
The
eastern
China
seas
are
highly
productive
with
significant
emissions
of
biogenic
substances,
but
spatiotemporal
variations
marine
aerosols
not
well
known.
Air
mass
exposure
chlorophyll
(AEC)
can
be
used
indicate
influence
sources
atmosphere
certain
degree.
In
this
study,
12
year
(2009-2020)
daily
AEC
were
calculated
over
seas,
showing
spatial
seasonal
patterns
intensity
which
co-controlled
by
surface
phytoplankton
biomass
boundary
layer
height.
By
combining
values,
relevant
meteorological
parameters,
extensive
observations
typical
secondary
aerosol
component,
methanesulfonate
(MSA),
parameterization
scheme
for
MSA
simulation
was
successfully
constructed.
This
AEC-based
approach
observation
constraints
provides
new
insight
into
distribution
aerosols.
Meanwhile,
wintertime
air
retention
land
exhibited
decrease,
decadal
weakening
trend
terrestrial
transport,
is
probably
related
East
Asian
winter
monsoon.
Thus,
may
play
an
increasingly
important
role
in
studied
region.
Journal of Geophysical Research Atmospheres,
Journal Year:
2023,
Volume and Issue:
128(20)
Published: Oct. 14, 2023
Abstract
Atmospheric
aerosol
particles
impact
Earth's
radiation
balance
by
acting
as
seeds
for
cloud
droplet
formation.
Over
half
of
global
seed
are
formed
nucleation,
a
process
where
gas‐phase
compounds
react
to
form
stable
particles.
Reactions
sulfuric
acid
(SA)
with
wide
variety
atmospheric
have
been
previously
shown
drive
nucleation
in
the
lower
troposphere.
However,
climate
models
poorly
predict
particle
rates
since
current
do
not
describe
systems
containing
tens
hundreds
precursor
compounds.
The
potential
model
(NPM)
was
recently
developed
SA
complex
mixtures
measuring
an
effective
base
concentration
using
1‐nm
condensation
counter.
This
technique
estimating
can
be
deployed
at
much
higher
spatial
and
temporal
resolution
than
methods
which
require
detailed
knowledge
all
reactions
measurements,
typically
mass
spectrometer,
gases.
work
expands
NPM
showing
that
this
capture
enhancement
suppression
within
mixture
organic
inorganic
acids,
ambient
air,
across
range
atmospherically
relevant
relative
humidities.
In
addition,
expression
calculating
also
derived
from
NPM.
Ultimately,
provides
simple
way
measure
extent
enhance
Physical Chemistry Chemical Physics,
Journal Year:
2024,
Volume and Issue:
26(11), P. 9005 - 9020
Published: Jan. 1, 2024
This
study
reports
on
the
high
yield
of
new
particle
formation
(NPF)
from
reaction
an
alkanolamine
commonly
used
in
carbon
capture
and
storage
technology,
monoethanolamine,
with
strong
atmospherically
relevant
acid,
methanesulfonic
acid.
Research Square (Research Square),
Journal Year:
2024,
Volume and Issue:
unknown
Published: March 11, 2024
Abstract
Natural
aerosols
are
an
important,
yet
understudied,
part
of
the
Arctic
climate
system.
marine
biogenic
aerosol
components
(e.g.,
methanesulfonic
acid,
MSA)
becoming
increasingly
important
due
to
changing
environmental
conditions.
In
this
study,
we
combine
in
situ
observations
with
atmospheric
transport
modeling
and
meteorological
reanalysis
data
a
data-driven
framework
aim
(1)
identify
seasonal
cycles
source
regions
MSA,
(2)
elucidate
relationships
between
MSA
variables,
(3)
project
response
based
on
trends
extrapolated
from
variables
determine
which
contributing
these
projected
changes.
We
have
identified
main
areas
be
Atlantic
Pacific
sectors
Arctic.
Using
gradient-boosted
trees,
were
able
explain
84
%
variance
find
that
most
for
indirectly
related
either
gas-
or
aqueous-phase
oxidation
dimethyl
sulfide
(DMS):
shortwave
longwave
downwelling
radiation,
temperature,
low
cloud
cover.
undergo
shift,
non-monotonic
decreases
April/May
increases
June-September,
over
next
50
years.
Different
different
months
driving
changes,
highlighting
complexity
influences
natural
component.
Although
oceanic
(sea
surface
DMS
emissions,
sea
ice)
precipitation
remains
seen,
here
show
will
likely
shift
solely
changes
variables.