Abstract.
In
this
study,
we
present
and
analyze
the
first
continuous
timeseries
of
relevant
aerosol
precursor
vapors
from
central
Arctic
during
Multidisciplinary
drifting
Observatory
for
Study
Climate
(MOSAiC)
expedition.
These
include
sulfuric
acid
(SA),
methanesulfonic
(MSA),
iodic
(IA).
We
use
FLEXPART
simulations,
inverse
modeling,
sulfur
dioxide
(SO2)
mixing
ratios,
chlorophyll-a
(chl-a)
observations
to
interpret
20
seasonal
variability
vapor
concentrations
identify
dominant
sources.
Our
results
show
that
both
natural
anthropogenic
sources
are
SA
in
Arctic,
but
associated
with
haze
most
prevalent.
MSA
an
order
magnitude
higher
polar
day
than
night
due
changes
biological
activity.
Peak
were
observed
May,
which
corresponds
timing
annual
peak
chl-a
north
75°
N.
IA
exhibit
two
distinct
peaks
25
year:
a
spring
secondary
autumn,
suggesting
depend
on
solar
radiation
sea
ice
conditions.
general,
cycles
SA,
MSA,
Ocean
related
conditions,
expect
environment
will
affect
these
future.
The
subsequent
influence
processes
remains
uncertain,
highlighting
need
continued
Arctic.
The
contribution
of
iodine-containing
compounds
to
atmospheric
new
particle
formation
is
still
not
fully
understood,
but
iodic
acid
and
iodous
are
thought
be
significant
contributors.
While
several
quantum
chemical
studies
have
been
carried
out
on
clusters
containing
iodine,
there
no
comprehensive
benchmark
study
quantifying
the
accuracy
applied
methods.
Here,
we
present
first
paper
in
a
series
that
investigate
role
iodine
species
cluster
formation.
In
this
work,
studied
monomers,
tetroxide
pentoxide
their
dimer
with
common
precursors.
We
tested
commonly
methods
for
calculating
geome-
try
thermal
corrections
monomers
dimers,
spin-orbit
coupling
finally
electronic
energy
correction
calculated
at
different
levels
theory.
find
optimizing
structures
either
ωB97X-D3BJ/aug-cc-pVTZ-PP
or
M06-2X/aug-cc-pVTZ-PP
level
achieves
best
binding
free
energy.
can
then
ZORA-DLPNO-CCSD(T0)
SARC-ZORA-TZVPP
basis
ma-ZORA-def2-TZVPP
non-iodine
atoms.
This
combination
yields
results
excellent
agreement
relativistic
calculations
comparatively
low
computational
cost.
methodology
calculate
energies
clusters,
where
confirm
qualitative
trends
observed
previous
studies.
However,
identify
overestimate
stability
by
kcal/mol
due
neglect
effects.
means
currently
nucleation
pathways
likely
overestimated.
Abstract.
In
this
study,
we
present
and
analyze
the
first
continuous
timeseries
of
relevant
aerosol
precursor
vapors
from
central
Arctic
during
Multidisciplinary
drifting
Observatory
for
Study
Climate
(MOSAiC)
expedition.
These
include
sulfuric
acid
(SA),
methanesulfonic
(MSA),
iodic
(IA).
We
use
FLEXPART
simulations,
inverse
modeling,
sulfur
dioxide
(SO2)
mixing
ratios,
chlorophyll-a
(chl-a)
observations
to
interpret
20
seasonal
variability
vapor
concentrations
identify
dominant
sources.
Our
results
show
that
both
natural
anthropogenic
sources
are
SA
in
Arctic,
but
associated
with
haze
most
prevalent.
MSA
an
order
magnitude
higher
polar
day
than
night
due
changes
biological
activity.
Peak
were
observed
May,
which
corresponds
timing
annual
peak
chl-a
north
75°
N.
IA
exhibit
two
distinct
peaks
25
year:
a
spring
secondary
autumn,
suggesting
depend
on
solar
radiation
sea
ice
conditions.
general,
cycles
SA,
MSA,
Ocean
related
conditions,
expect
environment
will
affect
these
future.
The
subsequent
influence
processes
remains
uncertain,
highlighting
need
continued
Arctic.
Abstract.
In
this
study,
we
present
and
analyze
the
first
continuous
timeseries
of
relevant
aerosol
precursor
vapors
from
central
Arctic
during
Multidisciplinary
drifting
Observatory
for
Study
Climate
(MOSAiC)
expedition.
These
include
sulfuric
acid
(SA),
methanesulfonic
(MSA),
iodic
(IA).
We
use
FLEXPART
simulations,
inverse
modeling,
sulfur
dioxide
(SO2)
mixing
ratios,
chlorophyll-a
(chl-a)
observations
to
interpret
20
seasonal
variability
vapor
concentrations
identify
dominant
sources.
Our
results
show
that
both
natural
anthropogenic
sources
are
SA
in
Arctic,
but
associated
with
haze
most
prevalent.
MSA
an
order
magnitude
higher
polar
day
than
night
due
changes
biological
activity.
Peak
were
observed
May,
which
corresponds
timing
annual
peak
chl-a
north
75°
N.
IA
exhibit
two
distinct
peaks
25
year:
a
spring
secondary
autumn,
suggesting
depend
on
solar
radiation
sea
ice
conditions.
general,
cycles
SA,
MSA,
Ocean
related
conditions,
expect
environment
will
affect
these
future.
The
subsequent
influence
processes
remains
uncertain,
highlighting
need
continued
Arctic.
Abstract.
In
this
study,
we
present
and
analyze
the
first
continuous
timeseries
of
relevant
aerosol
precursor
vapors
from
central
Arctic
during
Multidisciplinary
drifting
Observatory
for
Study
Climate
(MOSAiC)
expedition.
These
include
sulfuric
acid
(SA),
methanesulfonic
(MSA),
iodic
(IA).
We
use
FLEXPART
simulations,
inverse
modeling,
sulfur
dioxide
(SO2)
mixing
ratios,
chlorophyll-a
(chl-a)
observations
to
interpret
20
seasonal
variability
vapor
concentrations
identify
dominant
sources.
Our
results
show
that
both
natural
anthropogenic
sources
are
SA
in
Arctic,
but
associated
with
haze
most
prevalent.
MSA
an
order
magnitude
higher
polar
day
than
night
due
changes
biological
activity.
Peak
were
observed
May,
which
corresponds
timing
annual
peak
chl-a
north
75°
N.
IA
exhibit
two
distinct
peaks
25
year:
a
spring
secondary
autumn,
suggesting
depend
on
solar
radiation
sea
ice
conditions.
general,
cycles
SA,
MSA,
Ocean
related
conditions,
expect
environment
will
affect
these
future.
The
subsequent
influence
processes
remains
uncertain,
highlighting
need
continued
Arctic.
Abstract.
In
this
study,
we
present
and
analyze
the
first
continuous
timeseries
of
relevant
aerosol
precursor
vapors
from
central
Arctic
during
Multidisciplinary
drifting
Observatory
for
Study
Climate
(MOSAiC)
expedition.
These
include
sulfuric
acid
(SA),
methanesulfonic
(MSA),
iodic
(IA).
We
use
FLEXPART
simulations,
inverse
modeling,
sulfur
dioxide
(SO2)
mixing
ratios,
chlorophyll-a
(chl-a)
observations
to
interpret
20
seasonal
variability
vapor
concentrations
identify
dominant
sources.
Our
results
show
that
both
natural
anthropogenic
sources
are
SA
in
Arctic,
but
associated
with
haze
most
prevalent.
MSA
an
order
magnitude
higher
polar
day
than
night
due
changes
biological
activity.
Peak
were
observed
May,
which
corresponds
timing
annual
peak
chl-a
north
75°
N.
IA
exhibit
two
distinct
peaks
25
year:
a
spring
secondary
autumn,
suggesting
depend
on
solar
radiation
sea
ice
conditions.
general,
cycles
SA,
MSA,
Ocean
related
conditions,
expect
environment
will
affect
these
future.
The
subsequent
influence
processes
remains
uncertain,
highlighting
need
continued
Arctic.