Atmospheric chemistry and physics,
Journal Year:
2015,
Volume and Issue:
15(12), P. 6745 - 6765
Published: June 18, 2015
Abstract.
It
has
been
postulated
that
secondary
organic
particulate
matter
plays
a
pivotal
role
in
the
early
growth
of
newly
formed
particles
forest
areas.
The
recently
detected
class
extremely
low
volatile
compounds
(ELVOC)
provides
missing
vapors
and
possibly
contributes
significant
fraction
to
atmospheric
SOA
(secondary
aerosol).
sequential
rearrangement
peroxy
radicals
subsequent
O2
addition
results
ELVOC
which
are
highly
oxidized
multifunctional
molecules
(HOM).
Key
for
efficiency
such
HOM
particle
is
their
formation
induced
by
one
attack
oxidant
(here
O3),
followed
an
autoxidation
process
involving
molecular
oxygen.
Similar
mechanisms
were
observed
predicted
quantum
mechanical
calculations
e.g.,
isoprene.
To
assess
importance
therewith
potential
generality,
it
crucial
understand
pathway
HOM.
elucidate
path
as
well
necessary
sufficient
structural
prerequisites
we
studied
homologous
series
cycloalkenes
comparison
two
monoterpenes.
We
able
directly
observe
with
8
or
10
O
atoms
Atmospheric
Pressure
interface
High
Resolution
Time
Flight
Mass
Spectrometer
(APi-TOF-MS)
equipped
NO3−-chemical
ionization
(CI)
source.
In
case
O3
acting
oxidant,
starting
radical
on
so-called
vinylhydroperoxide
path.
termination
reactions
other
radicals,
including
dimerization,
allowed
analyzing
mass
spectra
narrowing
down
likely
As
consequence,
propose
percarboxylic
acids,
carbonyl,
hydroperoxy,
hydroxy
groups
arising
from
steps.
figured
aldehyde
facilitate
initial
simple
like
cycloalkenes,
was
limited
both
terminal
C
further
respective
α
positions.
more
complex
containing
tertiary
H
small,
constrained
rings,
even
higher
oxidation
degrees
possible,
either
shift
atom
initialization
ring-opening
reactions.
Proceedings of the National Academy of Sciences,
Journal Year:
2014,
Volume and Issue:
111(49), P. 17373 - 17378
Published: Nov. 24, 2014
Significance
We
illustrate
the
similarity
and
difference
in
particulate
matter
(PM)
formation
between
Beijing
other
world
regions.
The
periodic
cycle
of
PM
events
is
regulated
by
meteorological
conditions.
While
particle
chemical
compositions
are
similar
to
those
commonly
measured
worldwide,
efficient
nucleation
growth
over
an
extended
period
distinctive
from
aerosol
typically
observed
global
areas.
Gaseous
emissions
volatile
organic
compounds
nitrogen
oxides
urban
transportation
sulfur
dioxide
regional
industry
responsible
for
large
secondary
formation,
while
primary
transport
insignificant.
Reductions
precursor
gases
essential
mediate
severe
haze
pollution
China.
Chemical Reviews,
Journal Year:
2019,
Volume and Issue:
119(6), P. 3472 - 3509
Published: Feb. 25, 2019
Highly
oxygenated
organic
molecules
(HOM)
are
formed
in
the
atmosphere
via
autoxidation
involving
peroxy
radicals
arising
from
volatile
compounds
(VOC).
HOM
condense
on
pre-existing
particles
and
can
be
involved
new
particle
formation.
thus
contribute
to
formation
of
secondary
aerosol
(SOA),
a
significant
ubiquitous
component
atmospheric
known
affect
Earth's
radiation
balance.
were
discovered
only
very
recently,
but
interest
these
has
grown
rapidly.
In
this
Review,
we
define
describe
currently
available
techniques
for
their
identification/quantification,
followed
by
summary
current
knowledge
mechanisms
physicochemical
properties.
A
main
aim
is
provide
common
frame
quite
fragmented
literature
studies.
Finally,
highlight
existing
gaps
our
understanding
suggest
directions
future
research.
Global Environmental Change,
Journal Year:
2017,
Volume and Issue:
43, P. 51 - 61
Published: Feb. 9, 2017
Forest-driven
water
and
energy
cycles
are
poorly
integrated
into
regional,
national,
continental
global
decision-making
on
climate
change
adaptation,
mitigation,
land
use
management.
This
constrains
humanity’s
ability
to
protect
our
planet’s
life-sustaining
functions.
The
substantial
body
of
research
we
review
reveals
that
forest,
interactions
provide
the
foundations
for
carbon
storage,
cooling
terrestrial
surfaces
distributing
resources.
Forests
trees
must
be
recognized
as
prime
regulators
within
water,
cycles.
If
these
functions
ignored,
planners
will
unable
assess,
adapt
or
mitigate
impacts
changing
cover
climate.
Our
call
action
targets
a
reversal
paradigms,
from
carbon-centric
model
one
treats
hydrologic
climate-cooling
effects
forests
first
order
priority.
For
reasons
sustainability,
storage
remain
secondary,
though
valuable,
by-product.
tree
at
local,
regional
scales
offer
benefits
demand
wider
recognition.
forest-
tree-centered
insights
analyze
knowledge-base
improving
plans,
policies
actions.
understanding
how
influence
has
important
implications,
both
structure
planning,
management
governance
institutions,
well
might
used
improve
adaptation
mitigation
efforts.
Reviews of Geophysics,
Journal Year:
2017,
Volume and Issue:
55(2), P. 509 - 559
Published: May 18, 2017
Abstract
Anthropogenic
emissions
and
land
use
changes
have
modified
atmospheric
aerosol
concentrations
size
distributions
over
time.
Understanding
preindustrial
conditions
in
organic
due
to
anthropogenic
activities
is
important
because
these
features
(1)
influence
estimates
of
radiative
forcing
(2)
can
confound
the
historical
response
climate
increases
greenhouse
gases.
Secondary
(SOA),
formed
atmosphere
by
oxidation
gases,
represents
a
major
fraction
global
submicron‐sized
aerosol.
Over
past
decade,
significant
advances
understanding
SOA
properties
formation
mechanisms
occurred
through
measurements,
yet
current
models
typically
do
not
comprehensively
include
all
processes.
This
review
summarizes
some
developments
during
decade
formation.
We
highlight
importance
processes
that
growth
particles
sizes
relevant
for
clouds
forcing,
including
extremely
low
volatility
organics
gas
phase,
acid‐catalyzed
multiphase
chemistry
isoprene
epoxydiols,
particle‐phase
oligomerization,
physical
such
as
viscosity.
Several
highlighted
this
are
complex
interdependent
nonlinear
effects
on
properties,
formation,
evolution
SOA.
Current
neglect
complexity
nonlinearity
thus
less
likely
accurately
predict
project
future
sensitivity
Efforts
also
needed
rank
most
influential
process‐related
interactions,
so
be
represented
chemistry‐climate
models.
Atmospheric chemistry and physics,
Journal Year:
2015,
Volume and Issue:
15(14), P. 8217 - 8299
Published: July 24, 2015
Abstract.
The
literature
on
atmospheric
particulate
matter
(PM),
or
aerosol,
has
increased
enormously
over
the
last
2
decades
and
amounts
now
to
some
1500–2000
papers
per
year
in
refereed
literature.
This
is
part
due
enormous
advances
measurement
technologies,
which
have
allowed
for
an
increasingly
accurate
understanding
of
chemical
composition
physical
properties
particles
their
processes
atmosphere.
growing
scientific
interest
aerosol
high
importance
environmental
policy.
In
fact,
constitutes
one
most
challenging
problems
both
air
quality
climate
change
policies.
this
context,
paper
reviews
recent
results
within
sciences
policy
needs,
driven
much
increase
monitoring
mechanistic
research
decades.
synthesis
reveals
many
new
developments
science
underpinning
climate–aerosol
interactions
effects
PM
human
health
environment.
However,
while
airborne
responsible
globally
important
influences
premature
mortality,
we
still
do
not
know
relative
different
components
these
effects.
Likewise,
magnitude
overall
remains
highly
uncertain.
Despite
uncertainty
there
are
things
that
could
be
done
mitigate
local
global
PM.
Recent
analyses
shown
reducing
black
carbon
(BC)
emissions,
using
known
control
measures,
would
reduce
warming
delay
time
when
anthropogenic
temperature
exceed
°C.
cost-effective
measures
ammonia,
agricultural
precursor
gas
secondary
inorganic
aerosols
(SIA),
regional
eutrophication
concentrations
large
areas
Europe,
China
USA.
Thus,
environment
population.
A
prioritized
list
actions
full
range
currently
undeliverable
shortcomings
knowledge
science;
among
shortcomings,
roles
sources
response
land
use
remaining
century
prominent.
any
case,
evidence
from
strongly
advocates
integrated
approach
Nature,
Journal Year:
2016,
Volume and Issue:
533(7604), P. 527 - 531
Published: May 25, 2016
Abstract
About
half
of
present-day
cloud
condensation
nuclei
originate
from
atmospheric
nucleation,
frequently
appearing
as
a
burst
new
particles
near
midday
1
.
Atmospheric
observations
show
that
the
growth
rate
often
accelerates
when
diameter
is
between
one
and
ten
nanometres
2,3
In
this
critical
size
range,
are
most
likely
to
be
lost
by
coagulation
with
pre-existing
4
,
thereby
failing
form
typically
50
100
across.
Sulfuric
acid
vapour
involved
in
nucleation
but
too
scarce
explain
subsequent
5,6
leaving
organic
vapours
plausible
alternative,
at
least
planetary
boundary
layer
7,8,9,10
Although
recent
studies
11,12,13
predict
low-volatility
contribute
during
initial
growth,
direct
evidence
has
been
lacking.
The
accelerating
may
result
increased
photolytic
production
condensable
species
afternoon
2
presence
possible
Kelvin
(curvature)
effect,
which
inhibits
on
smallest
(the
nano-Köhler
theory)
2,14
so
far
remained
ambiguous.
Here
we
present
experiments
performed
large
chamber
under
conditions
investigate
role
nucleated
absence
inorganic
acids
bases
such
sulfuric
or
ammonia
amines,
respectively.
Using
data
same
set
experiments,
it
shown
15
alone
can
drive
nucleation.
We
focus
find
have
extremely
low
volatilities
(saturation
concentration
less
than
10
−4.5
micrograms
per
cubic
metre).
As
increase
barrier
falls,
primarily
due
more
abundant
slightly
higher
volatility
concentrations
−0.5
particle
model
quantitatively
reproduces
our
measurements.
Furthermore,
implement
parameterization
first
steps
global
aerosol
change
substantially
response,
is,
up
cent
comparison
previously
assumed
parameterizations.
Nature,
Journal Year:
2016,
Volume and Issue:
533(7604), P. 521 - 526
Published: May 25, 2016
Abstract
Atmospheric
aerosols
and
their
effect
on
clouds
are
thought
to
be
important
for
anthropogenic
radiative
forcing
of
the
climate,
yet
remain
poorly
understood
1
.
Globally,
around
half
cloud
condensation
nuclei
originate
from
nucleation
atmospheric
vapours
2
It
is
that
sulfuric
acid
essential
initiate
most
particle
formation
in
atmosphere
3,4
,
ions
have
a
relatively
minor
role
5
Some
laboratory
studies,
however,
reported
organic
without
intentional
addition
acid,
although
contamination
could
not
excluded
6,7
Here
we
present
evidence
aerosol
particles
highly
oxidized
biogenic
absence
large
chamber
under
conditions.
The
oxygenated
molecules
(HOMs)
produced
by
ozonolysis
α-pinene.
We
find
Galactic
cosmic
rays
increase
rate
one
two
orders
magnitude
compared
with
neutral
nucleation.
Our
experimental
findings
supported
quantum
chemical
calculations
cluster
binding
energies
representative
HOMs.
Ion-induced
pure
constitutes
potentially
widespread
source
terrestrial
environments
low
pollution.
Science,
Journal Year:
2018,
Volume and Issue:
361(6399), P. 278 - 281
Published: July 19, 2018
Atmospheric
new
particle
formation
(NPF)
is
an
important
global
phenomenon
that
nevertheless
sensitive
to
ambient
conditions.
According
both
observation
and
theoretical
arguments,
NPF
usually
requires
a
relatively
high
sulfuric
acid
(H2SO4)
concentration
promote
the
of
particles
low
preexisting
aerosol
loading
minimize
sink
particles.
We
investigated
in
Shanghai
were
able
observe
precursor
vapors
initial
clusters
at
molecular
level
megacity.
High
rates
observed
coincide
with
several
familiar
markers
suggestive
H2SO4-dimethylamine
(DMA)-water
(H2O)
nucleation,
including
dimers
H2SO4-DMA
clusters.
In
cluster
kinetics
simulation,
was
enough
explain
growth
~3
nanometers
under
very
condensation
sink,
whereas
subsequent
higher
rate
beyond
this
size
believed
result
from
added
contribution
condensing
organic
species.
These
findings
will
help
understanding
urban
its
air
quality
climate
effects,
as
well
formulating
policies
mitigate
secondary
China.