ACPAtmospheric Chemistry and PhysicsACPAtmos. Chem. Phys.1680-7324Copernicus PublicationsGöttingen, Germany10.5194/acp-17-13747-2017Particulate trimethylamine in the summertime Canadian high Arctic lower troposphereKöllnerFranziskaf.koellner@mpic.dehttps://orcid.org/0000-0002-4967-5514SchneiderJohanneshttps://orcid.org/0000-0001-7169-3973WillisMegan D.https://orcid.org/0000-0003-0386-0156KlimachThomasHelleisFrankBozemHeikohttps://orcid.org/0000-0003-2412-9864KunkelDanielhttps://orcid.org/0000-0002-9652-0099HoorPeterBurkartJuliaLeaitchW. RichardAliabadiAmir A.AbbattJonathan P. D.https://orcid.org/0000-0002-3372-334XHerberAndreas B.BorrmannStephanhttps://orcid.org/0000-0002-4774-9380Max Planck Institute for Chemistry, Mainz, GermanyInstitute for Atmospheric Physics, Johannes Gutenberg University Mainz, Mainz, GermanyDepartment of Chemistry, University of Toronto, Toronto, CanadaEnvironment and Climate Change Canada, Toronto, CanadaAlfred Wegener Institute for Polar and Marine Research, Bremerhaven, Germanynow at: Environmental Engineering Program, University of Guelph, Guelph, CanadaFranziska Köllner (f.koellner@mpic.de)20November20171722137471376631May20176June201711October201712October2017This work is licensed under the Creative Commons Attribution 3.0 Unported License. To view a copy of this licence, visit https://creativecommons.org/licenses/by/3.0/This article is available from https://acp.copernicus.org/articles/17/13747/2017/acp-17-13747-2017.htmlThe full text article is available as a PDF file from https://acp.copernicus.org/articles/17/13747/2017/acp-17-13747-2017.pdf
Size-resolved and vertical profile measurements of single
particle chemical composition (sampling altitude range 50–3000 m) were
conducted in July 2014 in the Canadian high Arctic during an aircraft-based measurement campaign (NETCARE 2014). We deployed the single particle laser ablation aerosol mass spectrometer ALABAMA (vacuum aerodynamic diameter range
approximately 200–1000 nm) to identify different particle types and their
mixing states. On the basis of the single particle analysis, we found that a
significant fraction (23 %) of all analyzed particles (in total: 7412)
contained trimethylamine (TMA). Two main pieces of evidence suggest that
these TMA-containing particles originated from emissions within the Arctic
boundary layer. First, the maximum fraction of particulate TMA occurred in
the Arctic boundary layer. Second, compared to particles observed aloft, TMA
particles were smaller and less oxidized. Further, air mass history analysis,
associated wind data and comparison with measurements of methanesulfonic acid
give evidence of a marine-biogenic influence on particulate TMA. Moreover,
the external mixture of TMA-containing particles and sodium and chloride
(“Na / Cl-”) containing particles, together with low wind speeds,
suggests particulate TMA results from secondary conversion of precursor gases
released by the ocean. In contrast to TMA-containing particles originating
from inner-Arctic sources, particles with biomass burning markers (such as
levoglucosan and potassium) showed a higher fraction at higher altitudes,
indicating long-range transport as their source. Our measurements highlight
the importance of natural, marine inner-Arctic sources for composition and
growth of summertime Arctic aerosol.
Introduction
A remarkable increase in Arctic near-surface air temperature
e.g., has led to rather drastic changes in
several climate parameters, in particular a decreasing sea ice extent of 3.5
to 4.1 % per decade since 1979 (, 2014, with
further evidence up to 2017 from the National Snow and Ice Data Center,
Boulder, Colorado, https://nsidc.org). Among the processes driving
Arctic warming, direct and indirect radiative effects of aerosol particles
play a key role. The impact of aerosol particles on the radiation budget
strongly depends on number concentration, size and chemical composition
e.g.,. Different measurements at Arctic sites show a
strong annual cycle in these aerosol characteristics
e.g.,. Three
main processes drive the annual cycle in Arctic aerosol. First, pollution
sources within the polar dome are reduced during summer, since the polar dome
surface extent is smaller during summer compared to winter
e.g.,. Second, efficient
wet removal processes in liquid clouds lead to a smaller condensation sink in
the summertime Arctic, in contrast to wintertime conditions
e.g.,. Third, the substantial change in duration of
daylight in Arctic summer leads to increased photochemical processes and
increased biological activity, which further result in a higher nucleation
potential
e.g.,.
To better understand the physical and chemical processes leading to a higher
nucleation potential and the frequent appearance of clouds in the summertime
Arctic, it is crucial to study emissions of the terrestrial and oceanic
biosphere. So far, a few studies have discussed the importance of
methanesulfonic acid (MSA), an oxidation product of dimethylsulfide emitted
from ocean biomass, to take part in aerosol chemistry in the Arctic
e.g.,. It
is further known that marine biota also release certain gas-phase amines,
such as trimethylamine (TMA), into the atmosphere
e.g.,, which
subsequently may contribute to aerosol chemistry. Numerous chamber, modeling
and field studies at southern latitudes
e.g., have
focused on sources, emission rates and gas-to-particle partitioning processes
of atmospheric amines. So far, this research has shown that amines may take
part in aerosol chemistry in several ways. These include acid–base reactions
to form aminium salts and dissolution in cloud droplets (owing to their high
water solubility) where subsequent acid–base reactions can occur in the
aqueous phase
e.g.,.
Amines compete with ammonia (NH3) in neutralizing acidic aerosol. The
base that is favoured by these reactions depends on several parameters, such
as acidity of the aerosol, Henry's law coefficient and the concentration of
both substances in the atmosphere e.g.,.
Amines further may take part in aerosol chemistry via gas-phase oxidation
processes, leading to the formation of species such as amides, nitramines and
imines. The resulting lower volatility products can go on to form secondary
organic aerosol (SOA) e.g.,.
Despite these considerable advances in studies of atmospheric amines, very
little is known about their abundance in Arctic regions.
reported marine influence on amino acids in Arctic
aerosol. Further particle measurements at Mace Head, Ireland, have shown the
presence of organic compounds, such as amines, in aerosol that originated in
polar marine air masses . Supplement
briefly mentioned the detection of particulate TMA at a coastal Alaskan site
in summer. However, our knowledge about the influence of amines on Arctic
aerosol number concentration, size and chemical composition remains
incomplete. Based on chamber studies of enhanced sulfuric acid nucleation
rates due to the presence of amines , some studies have
speculated that amines contribute to particle nucleation and growth in the
summertime Arctic . For this reason the
main objective of this research is to investigate emission sources and
aerosol chemistry processes of particulate TMA in the summertime Arctic. We
used aircraft-based single particle chemical composition measurements
conducted in the Arctic summer. In addition, we analyze concurrent data from
further aerosol and trace gas instruments as well as Lagrangian modeling
simulations from FLEXPART. This study provides an important opportunity to
advance our understanding of the strong biological control over summertime
Arctic aerosol.
Experimental and modeling sectionDescription of the sampling site and measurement platform
As one part of the NETCARE project (Network on Climate and Aerosols:
Addressing Key Uncertainties in Remote Canadian Environments), aircraft-based
measurements were deployed from Resolute Bay, Nunavut (Canada), during
4–21 July 2014. In this study, we focus on measurements made between
4 and 12 July 2014. The satellite image from 4 July 2014 shown in
Fig. presents sea ice and open water conditions around
Resolute Bay, which can be regarded as typical during 4–12 July. Six
research flights (around 20 flight hours) were performed during this time.
Flight tracks covered altitudes from 50 to 3000 m above continental as well
as marine (partly covered with sea ice) regions (Fig. ).
Three flights aimed to sample above two polynyas north of Resolute Bay.
Notably, the sea ice south-east of Resolute Bay and close to the ice edge in
Lancaster Sound was largely covered with melt ponds.
Satellite image (visible range from MODIS)
from 4 July 2014 showing sea ice and open water conditions around Resolute
Bay, in Lancaster Sound, Nares Strait and Baffin Bay. The red box indicates
the region expanded with flight tracks in Fig. . The image
is courtesy of NASA Worldview: https://worldview.earthdata.nasa.gov.
The instrument platform was the research aircraft Polar 6, a modified Basler
BT-67 maintained by Kenn Borek and operated by the Alfred Wegener Institute
for Polar and Marine Research . The aircraft was equipped
with instruments to measure meteorological state parameters and several trace
gases as well as aerosol particle number, size and chemical composition. In
general, aerosol instruments were connected to a forward-facing
near-isokinetic stainless steel inlet, which was followed by a 1-inch
stainless steel manifold inside the cabin. All instruments were connected to
the common inlet line system with 1/4-inch stainless steel tubing. Reactive
trace gases were measured via a second PTFA inlet line. Further detailed
information on the inlet and sampling strategy can be found in
, , and
.
Instrumentation
Number concentrations of particles greater than 5 nm in diameter
(Nd>5nm) were measured with a TSI 3787 water-based
ultrafine condensation particle counter (UCPC). Particle size distributions
of particles greater than 250 nm (Nd>250nm) were measured
using an optical particle counter from GRIMM (model 1.129 Sky-OPC).
Measurements of carbon monoxide (CO) were conducted with an Aerolaser
ultra-fast CO monitor (model AL 5002). Sub-micron bulk aerosol composition
was measured with an Aerodyne high-resolution time-of-flight aerosol mass
spectrometer (HR-ToF-AMS). Operation of the HR-ToF-AMS aboard Polar 6 during
NETCARE is described in . State parameters and
meteorological measurements were made using an AIMMS-20 from Aventech
Research Inc. Detailed information on measurement principles and instrument
calibrations are given in and .
Satellite image (visible range from MODIS) from
4 July 2014 with a compilation of flight tracks conducted during 4–12 July
2014 (indicated with different colors).
In order to provide information about the chemical composition of single
aerosol particles, the ALABAMA (Aircraft-based Laser Ablation Aerosol Mass
Spectrometer; ) was deployed
on the Polar 6 during NETCARE 2014. The basic measurement principle of the
ALABAMA is as follows: first, the particles enter the system through a
constant-pressure inlet. While ambient pressure changes, this device
(custom-made at the Max Planck Institute for Chemistry) maintains a constant
pressure in the following aerodynamic lens by varying the volume flow rate
into the instrument. A flexible orifice is either squeezed or relaxed,
depending on atmospheric pressure, by bottom and top plates that are
connected to a rotor. After passing through the inlet, particles are focused
into a narrow beam with the help of a Liu-type aerodynamic lens
. The focused particles are detected by two
light scattering signals (using 405 nm laser diodes and photo-multipliers)
allowing the determination of the size-dependent particle velocity. By
comparing these values with the velocity of manufactured monodisperse
polystyrene latex particles in five sizes ranging from 190 to 800 nm, we can
derive the particle vacuum aerodynamic diameter (dva). Next, the
particles enter the ablation and ionization region in the high-vacuum system.
The particles are ablated and ionized by a single triggered laser shot
(266 nm, frequency-quadrupled Nd:YAG laser). In the final step, cations and
anions produced by laser ablation are guided into a bipolar Z-ToF (Z-shaped
Time of Flight) mass spectrometer, which provides bipolar mass spectra of
individual particles. Due to limitations of the aerodynamic lens transmission
efficiency and the lower detection limit of the photo-multipliers, the
ALABAMA covers a particle size range from approximately 200 to 1000 nm.
FLEXPART Lagrangian particle dispersion model
FLEXPART (FLEXible PARTicle dispersion model (here: version 10.0)) is a
Lagrangian particle dispersion model e.g.,. For our
analysis, we used operational analysis data from the European Centre for
Medium-Range Weather Forecast (ECMWF) with 0.125∘ spatial and 3 h
time resolution. FLEXPART was operated in backward mode to provide potential
emission sensitivity (PES) maps, which are the response functions to tracer
releases from a receptor location. The value of the PES function is related
to the particles' residence time in the output grid cell (for more details
see Sect. 5 in ). We used such PES maps together
with sea ice and open ocean coverage derived from the satellite image in
Fig. to determine the total residence time of the
measured air mass above open water regions 3 days prior to sampling at
altitudes up to 340 m. The model output frequency was set up to 1 h and
0.125∘ spatial resolution.
Single particle spectra analysis
In total, 7412 particles were chemically analyzed (mass spectra produced) by
the ALABAMA during the study; 94 % of these spectra include size
information; 80 % of these spectra have dual polarity. Considering
the 20 % single-polarity spectra, potential reasons for the lack of
negative ions are discussed in the Supplement, Sect. 1. Briefly, it is likely
that single-polarity spectra are produced in high relative humidity (RH)
environments , in particular marine
environments .
The CRISP software package (Concise Retrieval of
Information from Single Particles) was used to perform m/z
(mass to ion charge ratio) calibration of particle mass spectra and peak area
integration as well as to classify particle mass spectra using ion markers
for different species . The marker method requires
knowledge of certain ion markers belonging to a certain substance as well as
knowledge of a certain marker threshold (ion peak area threshold). The
typical fragmentation pattern of a substance due to laser ablation is crucial
for defining the distinct ion markers. Fragmentation depends on laser
wavelength and energy. Ion markers of many species are already well known
from laboratory measurements with the ALABAMA and
additionally from the literature of other single particle mass
spectrometers (SPMSs) using the same ablation laser wavelength.
Table lists ion markers of substances used in this study
to identify the external and internal mixing states of particles. The
identification of ion markers m/z+59 and +58 for TMA by
was confirmed by additional laboratory measurements with
the ALABAMA (Supplement Sect. 2). To decide whether an ion signal is present, we used ion peak area thresholds
of 10 and 25 mV for positive and negative mass spectra, respectively. Both
thresholds are chosen as a conservative measure on the basis of signal
intensities of the non-occupied m/z values. Supplement Sect. 3 presents a
detailed explanation of ion peak area threshold determination.
Marker species (with abbreviations) and associated ion markers used
in this study. Further given are references (SPMS lab and field studies) used
for the assignment of ion markers as well as additional comments on marker
species and ions.
Marker species (abbreviation)Ion markersReferencesComments(lab/field studies)Trimethylaminem/z+59 ((CH3)3N+); +58 (C3H8N+)1/2,3,4Additionally examined in laboratory(TMA)measurements with the ALABAMA(Supplement Sect. 2)Sodium and chloridem/z+23 (Na+);5,6/7,2Sodium and chloride as indicators 5,8(Na / Cl)(at least two of the following ions)of sea spray particles+46 (Na2+), +62 (Na2O+), +63 (Na2OH+);(at least two of the following ions)Isobaric interference with MSA+81/83 (Na2Cl+), -35/37 (Cl-),at m/z-95-93/95 (NaCl2-)Elemental carbon(at least six of the following ions)6/2,9Except m/z-96 (C8-)(EC)m/z+36, +48, +60,…, +144 (C3-12+)due to the isobaric interference withand/orSO4-(at least six of the following ions)m/z-36, -48, -60,…, -144 (C3-12-)Levoglucosan(at least two of the following ions)10/11Levoglucosan as indicatorm/z-45 (CHO2-), -59 (C2H3O2-),of biomass burning (BB) particles12-71 (C3H3O2-)Potassiumm/z+39 (K+)6/2,9,13,14K-dominant SPMS spectra associated(K)with BB particles10,13,14,15Ammoniumm/z+18 (NH4+)9/2,6(NH4)Methanesulfonic acidm/z-95 (CH3O3S-)16/17Isobaric interference with PO4-(MSA)can be excluded due to missing ionsignal for PO3- at m/z-79Sulfate(at least one of the following ions)9/2,6(S)m/z-97 (HSO4-), -96 (SO4-)
The semicolons (;) used in the list of ion markers serve as
“and”. Given reference numbers are defined as follows:
1, 2,
3, 4,
5, 6,
7, 8,
9, 10,
11, 12,
13, 14,
15, 16,
17.
Results and discussionsMeteorological conditions during the NETCARE 2014 campaign
The measurement period during 4–12 July 2014 was characterized by generally
clear skies, calm wind speeds (Fig. ) and occasional
scattered to broken stratocumulus clouds due to
prevailing high-pressure influence in the Resolute Bay region. Based on low
CO mixing ratios, low aerosol number concentrations (Fig. )
and backward trajectory analysis, air masses measured in this period
experienced a weak mid-latitudinal influence and were mainly affected by
local emission sources (also denoted as “Arctic air mass period” in
). As shown in Fig. , our measurements
took place largely over remote areas, which are dominated by Arctic
vegetation, open water regions (e.g., polynyas, Lancaster Sound) and sea ice
coverage. Furthermore, seabird colonies were located close to the ice edge in
Lancaster Sound and are likely a source of ammonia .
Anthropogenic emissions might have affected our measurements, but are mainly
related to the sparse Arctic settlements and can be
ruled out by comparison with other tracers (e.g., CO). We can therefore
expect that our observations from 4–12 July 2014 were mainly influenced by
Arctic marine and terrestrial emissions.
As is evident from vertical profiles of equivalent potential temperature
(Θe) (Fig. ), the mean upper boundary
layer (BL) height for this measurement period was at around
340 ± 100 m. The vertical resolution of the profile in
Fig. (100 m) justifies the range of the mean BL height.
The mean BL height within its range can be confirmed by results from an
extensive study on BL height, mixing and stability during the NETCARE 2014
campaign . The capping temperature inversion above
390 m, inferred from values of Θe, represents a transport
barrier for air masses between the BL and the free troposphere (FT). The BL,
compared to the FT, was characterized by lower wind speeds, higher RH and
enhanced Nd>5nm in contrast to
Nd>250nm, indicating an enhanced number of
ultrafine particles due to nucleation in the Arctic BL. A detailed discussion
of this topic is given in .
Size-resolved and vertically resolved aerosol composition
Applying the marker method (Sect. ), we classified 6676
particle mass spectra (90 % of the mass spectra analyzed by the
ALABAMA (Sect. )) into five distinct particle types: TMA-,
Na / Cl-, EC-, levoglucosan- and K-containing particles. TMA-,
levoglucosan- and K-containing particles, with relative fractions of 23, 18
and 46 %, respectively, appear to be the most prominent particle
types. Other alkylamines (other than TMA) and amino acids could not be
identified (Supplement Sect. 4). Furthermore, only 2 and 1 % of all
analyzed particles are assigned as EC- and Na / Cl-containing particles,
respectively. To obtain 100 % as the total particle number, every
spectrum is classified into one distinct particle type in the order presented
in Table . The mean spectra in Fig.
combined with the additional ion signals listed in Table
provide an overview of the average chemical composition of each particle
type; 28 and 9 % of TMA- and K-containing particle spectra lack
negative ions, respectively. Potential reasons for the lack of negative ions
are discussed in the Supplement, Sect. 1. The mean spectrum of the remaining
736 particles (10 % of mass spectra analyzed by the ALABAMA), which
could not be classified into one of the five particle groups outlined above,
is shown in Fig. S7 in the Supplement. For further analysis we summarize
these remaining particles in “others”.
Vertically resolved median (black line) and
interquartile ranges (gray shaded area) of the equivalent potential
temperature (Θe), relative humidity (RH), wind speed,
particle number concentration measured by the UCPC
(Nd>5nm) and Sky-OPC
(Nd>250nm) as well as the CO mixing ratio
(including all conducted flights from 4–12 July 2014). Measurements of
Nd>250nm started on 8 July due to prior technical
issues. The red line depicts the derived mean upper height of the boundary
layer during this measurement period (approximately 340 m).
In order to describe the unique characteristics of TMA-containing particles
compared to other particle groups, Figs. and
depict the size and vertical distribution of each particle type,
respectively. Both figures show the fractional abundance of each particle
type per size and altitude bin, respectively. We show relative numbers of
particles in order to eliminate the size-dependent transmission and detection
efficiency of the ALABAMA (Fig. ) and the dependence of the
number of detected particles on sampling time at different altitudes
(Fig. ). The following use of the word fraction always
refers to the number fraction measured by the ALABAMA.
Bipolar mean spectra of the identified
particle types: (a) TMA-containing (1688 particles =^
23 %), (b) Na / Cl-containing (106 particles
=^ 1 %), (c) EC-containing (138 particles =^ 2 %), (d) levoglucosan-containing
(1312 particles =^ 18 %) and (e) K-containing
(3432 particles =^ 46 %).
Overview of the obtained five particle types and their internal
mixing state derived from the mean spectra in Figs. and
. Additional ion signals of sulfate (m/z-97/99
(HSO4-), -96 (SO4-)) and potassium (m/z+39/41
(K+)) were present in every mean spectrum and have therefore not
been listed here. Further given are references (SPMS lab and field studies)
used for the assignment of the additional ion signals to the corresponding
chemical species.
Given reference numbers are defined as follows:
1,
2,
3,
4,
5,
6,
7,
8,
9,
10,
11.
Cumulative size-resolved aerosol composition of
the identified particle types (normalized to the total number of particles
analyzed by the ALABAMA (indicated by red dots)): TMA-containing (yellow),
Na / Cl-containing (blue), EC-containing (black),
levoglucosan-containing (brown), K-containing (green) and others (gray). The
errors associated with number fractions of the identified particle types were
calculated using binomial statistics.
Cumulative vertically resolved aerosol composition
of the identified particle types (normalized to the total number of particles
analyzed by the ALABAMA (indicated by red bars)): TMA-containing (yellow),
levoglucosan-containing (brown), Na / Cl-containing (blue),
EC-containing (black), K-containing (green) and others (gray). There are in
general two levels (below 340 m and above 2700 m) with an enhanced number
of particles analyzed by the ALABAMA, which is caused by a longer sampling
time within these altitudes.
Expanded mean anion spectrum of 106
(1 %) Na / Cl-containing single particle spectra from
Fig. b. Only the organics peaks are highlighted here.
Levoglucosan-, EC- and K-containing particle types
Levoglucosan, EC and potassium are known to be primarily produced from fossil
fuel and biomass combustion processes
e.g.,. In
particular, levoglucosan is formed via the breakdown of cellulose during
biomass burning processes. The size distributions of levoglucosan- and
EC-containing particles are shifted towards larger diameters compared to
other particle types (Fig. ). This result suggests these
particles were exposed to chemical aging during long-range transport from
biomass burning sources. K-containing particles are more evenly distributed
across the size distribution (280–970 nm). EC-, levoglucosan- and
K-containing particles contain mixtures of sulfate (m/z-97/99
(HSO4-)), MSA (m/z-95 (CH3SO3-)) and organic
nitrogen compounds (m/z-26 (CN-), m/z-42 (CNO-))
(Fig. c–e and Table ). Further, given
that the K+ ion signals (m/z+39/41) are dominant in mean cation
spectra (Fig. c–e), we can likely attribute these
particles to a biomass burning source
e.g.,. Furthermore,
assigned negative ion signals at m/z-73
(C3H5O2-) to glyoxylic acid, which is typically present in
biomass burning related SPMS spectra. analyzed biomass
burning particles internally mixed with oxalic acid (m/z-89
(C2O4H-)). Both peaks are present in EC and levoglucosan mean
mass spectra (Fig. c, d and Table ).
Previous Arctic SPMS studies by and
reported a particle type similar to our EC-containing particles (denoted as
ECOC type 1 and soot, respectively). attributed this
particle type to remote biomass/biofuel sources of continental origin. In
contrast, assigned a large fraction of soot particles to
emissions from the nearby oil fields at Prudhoe Bay. In the present study,
the remote location of Resolute Bay excludes a large influence of oil and
gas extraction activities . Further,
analyzed a particle type similar to the K-containing type
in this study and denoted as a K–CN–sulfate type. They have speculated
about a marine origin of these mixtures of potassium, sulfate and organic
nitrogen fragments. Sodium and MSA were partially present in the K-containing
particle type in our study (Fig. e and
Table ), which confirms the hypothesis of
. However, it is likely that this large group of
K-containing particles (46 %) includes different emission sources
inside and outside the local BL.
The vertical dependence in EC-containing particles is not further analyzed
here due to the low statistical significance of 138 particles detected over
the entire study at all altitudes. From the vertical profile of levoglucosan-
and K-containing particles given in Fig. , it can be seen that
their fractions increase with increasing altitude. These observations
correspond to enhanced CO mixing ratios and
Nd>250nm (Fig. ), providing
further evidence for biomass burning as the source of levoglucosan- and
K-containing particles. Despite the potential for oxidation of levoglucosan
during transport, it has been previously reported as associated with biomass
burning aerosol in Arctic regions .
and did not report the detection of
levoglucosan with SPMS measurements in the summertime Arctic. It is likely
that these ground-based measurements missed a large fraction of particles
typically present above the BL (including levoglucosan particles).
Na / Cl-containing particle type
A number of studies have reported on the primary production of sea spray
particles via bubble bursting at the sea surface
e.g.,. Na / Cl-containing particles
observed in this study show particle diameters mainly larger than 600 nm,
and they primarily exist at the lowest altitudes. Thus, the
Na / Cl-containing particle type can be associated with locally emitted
sea spray. The occurrence of sulfate and nitrate ion signals in the mean
spectrum (Fig. b and Table ) suggests
that some particles have already been exposed to chemical aging via reactions
with sulfuric and nitric acid forming nitrate and sulfate and releasing
HCl to the gas phase e.g.,.
Similar ion peaks were observed by and
and assigned to aged sea spray particles. Internal mixing of
Na / Cl-containing particles with MSA cannot be finally ruled out since
NaCl2- and MSA have an isobaric interference at m/z-95
(Table ). However, due to the concurrent existence of
other Na and Cl ion signals as well as signals at m/z-93 (isotope of
NaCl2-), it is likely that ion signals at m/z-95 are largely
produced by NaCl2-.
Interestingly, some of the Na / Cl-containing particles are internally
mixed with different inorganics (such as magnesium and calcium) as well as
oxygen- and nitrogen-containing organic compounds, as indicated by the mean
spectrum in Figs. b and . It is known
from previous SPMS laboratory studies on sea spray particles produced from
biologically active waters that organic nitrogen species present in inorganic
salts arise from biological activity . In
particular, organic nitrogen fragments together with calcium, sodium and
phosphate have been linked to signatures of biological species
e.g.,. SPMS spectra of biological particles
presented in further indicate the occurrence of
oxygen-containing organic compounds at m/z-71 (C3H3O2-).
Laboratory studies with the ALABAMA investigating biological species (such as
bacteria and pollen) also showed the existence of negative ion signals at
m/z-45 (C2H5O-), m/z-59
(C2H3O2-/C3H9N-) and m/z-71
(C3H3O2-/C4H7O-) in addition to the presence of
phosphate and organic nitrogen compounds . Anion signals
at m/z-26 (C2H2-) and m/z-42
(C2H2O-/C3H6-) can be further attributed to
cellulose . Moreover, reported the
concurrent presence of sodium, chloride and oxygen-containing organic
compounds (m/z-73 (C3H5O2-) and m/z-59
(C2H3O2-)) in ambient SPMS spectra and attributed them to
organic-containing sea salt particles. Other non-SPMS studies (e.g., X-ray
microscopy methods) have reported the occurrence of organic-rich (e.g.,
carboxylate) sea spray particles originating from microorganisms and organic
compounds enriched in the sea surface microlayer in mid-latitude oceans
e.g., and in Arctic regions
e.g.,. Taken
together, the presence of magnesium and calcium together with nitrogen- and
oxygen-containing organic species in sea spray particles suggests that such
organic fragments have a marine-biogenic origin.
TMA-containing particle type
TMA-containing particles have several characteristics that contrast with the
other particle types. The size distribution of TMA-containing particles is
shifted towards smaller diameters (Fig. ) and the fractional
abundance increases with decreasing altitude (Fig. ). In
addition, TMA-containing particles detected within the BL are smaller
compared to particles observed aloft (Fig. S8 in the Supplement). Comparison
of HR-ToF-AMS estimated oxygen-to-carbon (O / C) and hydrogen-to-carbon
(H / C) ratios with the ALABAMA particulate TMA fraction gives an
indication of the degree of particle oxidative aging
e.g.,. Less oxygenated
organics measured with the HR-ToF-AMS were present when the fraction of
TMA-containing particles was high (Fig. a, up to
75 % in the upper left corner). This suggests that a large fraction
of particulate TMA, especially within the BL (indicated with green circles in
Fig. b), had not been subject to extensive oxidative
aging. According to these results together with the existence of a stable
stratified BL (Fig. ), we can infer that particulate TMA
present within the Arctic BL originated from inner-Arctic sources. Possible
inner-Arctic sources of TMA, referring to , are oceanic
phytoplankton biomass or other marine organisms and various human activities
(e.g., waste incineration, vehicle exhaust, residential heating). Gaseous TMA
emissions may then take part in aerosol chemistry in several ways, including
acid–base reactions, oxidation processes, dissolution in cloud droplets and
nucleation
e.g.,.
The mean spectrum of TMA-containing particles (Fig. a)
shows no indications that further N-containing compounds (such as amine
oxidation products, e.g., amides, nitramines and imines) other than TMA (with
specific ion signals at m/z+59 and +58) were present in these particles.
Figure a and Table further illustrate
an internal mixing of sulfate and TMA, which indicates that aminium sulfate
salts may be present e.g.,. We
can therefore hypothesize that the formation of particulate TMA was
accompanied by acid–base reactions including TMA, sulfuric and
methanesulfonic acid e.g.,.
reported enhanced gas-to-particle partitioning of TMA by dissolution in
cloud/fog droplets and subsequent formation of aminium salts. Thus, it is
further possible, due to the occasional presence of low-level clouds
, that the formation of TMA-containing particles was
favored by pre-existing wet and acidic particles.
Comparison between the HR-ToF-AMS estimated
oxygen-to-carbon (O / C) and hydrogen-to-carbon (H / C) ratios
colored by (a) TMA-containing particle number fraction (ALABAMA) and
(b) total number of analyzed particles by the ALABAMA (gray to
black) as well as the presence of particulate TMA above (blue circles) and
below (green circles) 340 m (mean upper BL height, Sect. ).
Classification of TMA-containing particles
on the basis of their different internal mixing states. Each branch describes
the existence or non-existence of several substances (potassium (K),
ammonium (NH4), MSA and sulfate) on TMA-containing particles with
relative abundances normalized to the occurrence of 1688 TMA-containing
particles. An initial query regarding the existence of dual-polarity spectra
is included. Based on this classification, four TMA-containing particle
sub-types arise (colored boxes with relative fractions):
“K,NH4,MSA,S-”, “K,NH4,S-”, “K-” and
“Non-K,NH4-containing”. We further considered an internal mixing of
particulate TMA with levoglucosan (7 %), Na / Cl and EC (not
listed here), whereby the latter two types with relative fractions of less
than 1 % are negligible for further analysis. Gray-shaded numbers
indicate groups with relative fractions of less than 7 % that are
not further considered.
Internal mixing state of TMA-containing particles
The internal mixing state of TMA-containing particles was further classified
by applying the marker method introduced in Sect. and
Table for compounds that are apparent in the mean
spectrum (Fig. a and Table ), such as
potassium (K), ammonium (NH4), MSA and sulfate (S). The
diagram in Fig. illustrates the classification
algorithm as follows: an upper branch always refers to a positive response
(“yes”) for whether different ion markers are present in spectra or not; a
lower branch shows the opposite answer (“no”). Besides the substances that
already appeared in the mean spectrum of TMA-containing particles, here
TMA-containing spectra are also viewed based on the concurrent existence of
levoglucosan, Na / Cl and EC. We did not consider in detail the
concurrent existence of carbon cluster ions (m/z+12, +24,…),
different hydrocarbons (m/z+27 and +37) and oxidized organics (m/z+43)
since 90 % of all TMA-containing particles contain at least one of
these ion signals. The classification of the TMA-containing particle type is
further based on an initial differentiation between dual- and single-polarity
mass spectra. As can be seen in Fig. , 28 %
of TMA-containing particle spectra lack negative ions. Consequently, we
cannot state whether species producing anions (such as MSA and sulfate) were
present in these particles. Potential reasons for the lack of negative ions
are discussed in the Supplement Sect. 1. Particle sub-group notation is based
on the existence or non-existence of different species in TMA-containing
particles. For reasons of clarity, particle types with less than 7 %
fractional abundance (corresponding to a total number of less than 118
particles) are not explicitly considered in this analysis, but are summarized
as “others”. Following the categorization in Fig. ,
five groups of different internal mixing states arise: “K,NH4,MSA,S-”,
“K,NH4,S-”, “K-”, “Non-K,NH4-” and
“levoglucosan-containing” particles. These five TMA particle sub-types will
be divided into those containing biomass burning tracers (such as
levoglucosan and potassium) and those not containing these tracers.
Cumulative size-resolved aerosol composition
of TMA-containing particle sub-types (normalized to the total number of
TMA-containing particles (indicated by red dots)):
“K,NH4,MSA,S-containing” (dark green), “K,NH4,S-containing”
(light green), “K-containing” (orange), “Non-K,NH4-containing”
(yellow), “levoglucosan-containing” (brown) and “others” (light yellow).
Cumulative vertically resolved aerosol
composition of TMA-containing particle sub-types (normalized to the total
number of TMA-containing particles (indicated by red bars)):
“K,NH4,MSA,S-containing” (dark green), “K,NH4,S-containing”
(light green), “K-containing” (orange), “Non-K,NH4-containing”
(yellow), “levoglucosan-containing” (brown) and “others” (light yellow).
As can be seen in Fig. , a large fraction of
TMA-containing particles (74 %) are additionally composed of biomass
burning tracers such as potassium (67 %) and levoglucosan
(7 %). According to , this internal mixture can
be explained by potassium-containing particles acting as seeds for the
condensation of organic material. Thus, the measured particulate TMA can be
considered a secondary component that condensed on pre-existing primary
particles. It is also conceivable that TMA particles containing potassium and
levoglucosan are a result of biomass burning emissions
. The
size distribution of the TMA particles containing levoglucosan is shifted
towards larger diameters compared to other TMA particle sub-types
(Fig. ). Moreover, Fig. demonstrates
that TMA particle sub-types including potassium and levoglucosan were more
abundant above the BL, in contrast to “Non-K,NH4-containing” TMA
particles. Comparison between CO mixing ratios and TMA sub-types abundance
(Fig. ) shows larger fractions of “K,NH4,S-containing” and
“levoglucosan-containing” TMA particle sub-types in higher CO environments
compared to “Non-K,NH4-containing” TMA particles. Taken together,
these results suggest that TMA particles containing levoglucosan and
potassium likely originated from remote biomass burning emission sources and
were transported to our measurement site.
CO measurements compared with the cumulative fraction
of TMA-containing particle sub-types (normalized to all TMA-containing
particles (indicated by red dots)): “K,NH4,MSA,S-containing” (dark
green), “K,NH4,S-containing” (light green), “K-containing” (orange),
“Non-K,NH4-containing” (yellow), “levoglucosan-containing” (brown)
and “others” (light yellow).
Mean spectra of the
“Non-K,NH4-containing” TMA particle sub-type: (a)
single-polarity particle mass spectrum (12 %, yellow box in
Fig. ), (b) dual-polarity particle mass
spectrum (6 %, not colored in Fig. ).
Another large fraction (25 %, Fig. ) of
particulate TMA is neither internally mixed with potassium nor with any other
tracer of biomass burning. This result suggests that these TMA-containing
particles resulted from SOA formation. This is consistent with results from
particle size distributions of TMA sub-types in Fig.
illustrating that the fractional abundance of “Non-K,NH4-containing”
TMA particles is highest between 280 and 380 nm compared to other sub-types
containing levoglucosan and/or potassium. In particular, positive ion mass
spectra of the sub-type “Non-K,NH4-containing” (12 % single
polarity (yellow box in Fig. ) and 6 % dual
polarity (not colored in Fig. )) show ion signals
only for carbon cluster ions and fragments of hydrocarbons
(Fig. a, b). Due to a suppression of anion signals,
likely in high RH environments (Supplement Sect. 1), we cannot state whether
sulfate or MSA was present in these particles. However, the dual-polarity
mean spectrum of the 6 % TMA-containing particles not including
potassium and ammonium (Fig. b, not colored in
Fig. ) indicates the concurrent presence of sulfate
or MSA. From the absence of ammonium in these TMA particles containing
sulfate or MSA, we can further conclude that aminium salts were present. This
result demonstrates that amines, in addition to ammonia, may take part in the
neutralization of acidic aerosol. This is of particular interest considering
the reduced sources of ammonia in the Arctic and the ocean as a net sink of
NH3 in the summertime Canadian Arctic .
Furthermore, Fig. indicates a positive correlation between MSA
mass concentrations measured with HR-ToF-AMS and the fraction of
“Non-K,NH4-containing” TMA particles. Given that MSA can be used as an
indicator of marine influence on sub-micron aerosol, we can conclude that the
existence of an inner-Arctic marine-biogenic source of TMA is likely.
Moreover, “Non-K,NH4-containing” TMA particles are most abundant at
the lowest altitudes (Fig. ) and are coincident with the
presence of less aged particulate organic aerosol (Fig. ).
Taken together, the characteristics of the “Non-K,NH4-containing” TMA
particle sub-type suggest that gaseous TMA emissions from inner-Arctic
sources (likely marine-biogenic) act as precursors for the formation of SOA
within the summertime Arctic BL.
MSA concentrations measured with the HR-ToF-AMS
compared with the cumulative fraction of TMA-containing particle sub-types
(normalized to all TMA-containing particles (indicated by red dots)):
“K,NH4,MSA,S-containing” (dark green), “K,NH4,S-containing”
(light green), “K-containing” (orange), “Non-K,NH4-containing”
(yellow), “levoglucosan-containing” (brown) and “others” (light yellow).
Temporally resolved aerosol composition of the
identified non-TMA-containing particle types (normalized to the total number
of particles analyzed by the ALABAMA): Na / Cl-cont. (blue),
EC-cont. (black), levoglucosan-cont. (brown), K-cont. (green) and
“others” (gray) as well as TMA-containing particle sub-types (normalized to
the total number of particles analyzed by the ALABAMA):
“levoglucosan-cont.” (light brown), “K,NH4,MSA,S-cont.” (dark
green), “K,NH4,S-cont.” (light green), “K-cont.” (orange),
“Non-K,NH4-cont.” (yellow) and “others” (light yellow). Fractional
abundances of the particle types were calculated for 10 min time intervals.
Only time intervals with at least 20 measured particles were considered.
Measurements within the BL on 5, 10 and 12 July did not provide any 10 min
time interval with more than 20 spectra.
Spatially resolved fraction of TMA-containing
particles (a, color-coded) and wind direction (b,
color-coded) below 340 m. Different rows present different measurement days.
The first graph additionally shows the satellite image on 4 July in the
visible range. Further satellite images are not presented here due to
negligible changes in sea ice coverage from 4–8 July. Abbreviations N, E,
S and W refer to north, east, south and west. The black triangle presents the
location of Resolute Bay on the map.
FLEXPART backward simulations of the considered
measurement periods (Fig. ) 3 days prior to sampling and at
altitudes below 340 m. The color-coded area presents values of the potential
emission sensitivity (PES) function in a particular grid cell
(Sect. ). Different rows depict different measurement days.
Source apportionment analysis of TMA-containing particles
This section will further explore potential emission sources of TMA in the
Arctic BL. Thus, the following analysis was restricted to measurements below
340 m (mean upper BL height, Sect. ). Figure shows
the temporal distribution of non-TMA-containing particles (such as
Na / Cl-, EC-, levoglucosan- and K-containing) and TMA-containing
sub-types. Figure depicts the spatially resolved fraction of
TMA-containing particles below 340 m (left panel) as well as the measured
wind direction (right panel) for measurements on 4, 7 and 8 July. We further
used 3-day FLEXPART backward simulations (Sect. ) for air
mass history analysis of the three measurement legs (Fig. )
to understand the source regions of TMA-containing particles.
Potential emission sensitivity (PES) maps combined with sea ice coverage
(Fig. ) show that air masses measured on 4 and 7 July
spent less than 1 h and around 7 h, respectively, in the previous 3 days in
regions of open water (polynyas north of Resolute Bay and Nares Strait). On
both days the air was mainly advected above sea ice and snow covered regions
north of Resolute Bay (Fig. compared with
Fig. ). The prevailing wind direction on 4 and 7 July
along the flight tracks (Fig. ) is from the north and east and
therefore consistent with FLEXPART backward simulations
(Fig. ). From measurements on 4 and 7 July it is not
possible to attribute TMA emissions to marine-biogenic or anthropogenic
sources (e.g., vehicle exhaust, residential heating and waste incineration
emissions in Resolute Bay). A more detailed air mass history analysis was
carried out on observations from 8 July.
The case of 8 July provides further evidence for a marine-biogenic influence
on TMA-containing particles through secondary processes. The prevailing wind
direction along the presented flight leg is from the east
(Fig. ), with low wind speeds up to a maximum of
7 m s-1 (Fig. S9 in the Supplement). The fraction of TMA-containing
particles decreases with a shift to a more southerly wind direction (yellow
to green colors, Fig. ). The highest fractional abundance of
particulate TMA was measured close to the ice edge (Fig. ) at
low wind speeds close to 0 m s-1 (Fig. S9 in the Supplement). Thus,
the ice edge in the western section of Lancaster Sound where the highest
surface phytoplankton production rate and chlorophyll a
concentration were measured (M. Gosselin, personal communication,
2017) and large bird colonies at Prince Leopold Island
(Fig. ) likely contribute to TMA
emissions in the area. Consistent with these observations, previous aerosol
chemical composition measurements on Bird Island in the South Atlantic
(> 50∘ S) have reported the presence of amines and amino acids
emitted from local fauna, including seabirds, penguins and fur seals
. Further, air mass history predicted by FLEXPART 3-day
backward simulations (Fig. ) illustrates that these air
masses were advected at low levels above open water regions in Lancaster
Sound, Baffin Bay and Nares Strait (compare with
Fig. ). Air masses measured during this flight leg on
8 July resided for more than 17 h during the 3 days prior to sampling above
regions of open water. Further, anthropogenic influences on amine emissions
from nearby Resolute Bay are likely negligible since CO concentrations are
very low. Another important finding is that primary sea spray particles
(Na / Cl-containing) and TMA-containing particles measured on 8 July are
externally mixed (Fig. ), although both substances seem to be
released from the ocean. This analysis solidifies the earlier hypothesis
(Sect. ) that particulate TMA presents secondary aerosol
. The higher abundance of the TMA-containing particle
sub-type “Non-K,NH4-containing” on 8 July (Fig. ),
compared to other days, further supports the hypothesis of SOA formation. It
is further relevant to discuss that on 8 July from 15:50 until 17:20 UTC
(respective flight leg in Fig. ) we flew low over sea ice in the
vicinity of dissipating low-level clouds. These clouds had formed above the
open water regions east of our flight leg
. We can therefore assume that cloud
processing likely contributed to enhanced gas-to-particle partitioning of TMA
as earlier reported in . In addition, high
organic-to-sulfate and MSA-to-sulfate ratios measured with the HR-ToF-AMS
during this flight leg (see Sect. 4.3 in ) indicate that
particle growth was driven by ocean-derived precursor gases (dimethylsulfide
and organic species). Taken together, results from 8 July demonstrate
secondary organic aerosol formation from marine-biogenic sources of gas-phase
precursors, including TMA.
Conclusions
We presented results from aircraft-based single particle aerosol measurements
in the summertime Canadian high Arctic. Our study has shown the presence of
particulate TMA in the Arctic summer, comprising 23 % of all
particles analyzed by the ALABAMA. SPMS measurements do not provide bulk
analysis of aerosol chemical composition; therefore, we
cannot
obtain TMA mass concentrations. Nevertheless, the number of particles
analyzed by the ALABAMA (> 7000) is sufficient to conduct a statistical
analysis. This allows us to draw conclusions about mixing state, vertical and
size distributions as well as potential emission sources of particulate TMA
in summertime Arctic regions.
We present two main sources of particulate TMA in the summertime Arctic.
First, we show the presence of inner-Arctic marine-biogenic sources resulting
in secondary aerosol formation by TMA, sulfate, MSA, ammonia and other
organics. Second, we have indications of long-range transport from biomass
burning sources. We measured the maximum occurrence of particulate TMA
(approximately 60 %) in a clean and stable stratified Arctic BL. In
addition, TMA-containing particles present within the Arctic BL were smaller
and were associated with less aged organic aerosol compared to aerosol
observed aloft. High fractions of particulate TMA were measured at low wind
speeds (near 0 m s-1) and close to the biologically active marginal
ice zone. Further, BL air masses including high fractions of particulate TMA
spent a long time (more than 17 h) prior to sampling above Arctic open water
regions. Moreover, the TMA particle sub-type containing MSA, sulfate and
other organic species was more abundant when MSA mass concentrations
(measured with HR-ToF-AMS) were high. Furthermore, the concurrent existence
of sulfate, MSA and TMA in single particle spectra indicates the presence of
aminium salts. This demonstrates that TMA may take part in neutralizing
acidic aerosol along with ammonia. We additionally found that primary sea
spray particles and TMA-containing particles are externally mixed, although
both substances are released by the ocean. It is further possible that
gas-to-particle partitioning of TMA was enhanced in the vicinity of clouds
and fog through dissolution of TMA in droplets and subsequent acid–base
reactions . In contrast to the marine inner-Arctic
sources, we have evidence for particulate TMA from long-range transport of
biomass burning aerosol. We demonstrate that levoglucosan and potassium
(biomass burning tracers) are internally and externally mixed with
particulate TMA. These particle types were more abundant above the Arctic BL
as well as larger in particle sizes compared to particles not including these
components.
Taken together, these findings contribute to our knowledge of marine-biogenic
influences on secondary aerosol chemical composition and particle growth in
the summertime Canadian Arctic. This is the first study demonstrating the
incorporation of amines in Arctic aerosol from inner-Arctic sources. Based on
spatial and temporal limitations of our measurements, it is difficult to
assess how representative our findings are of the broader Arctic region.
However, recent measurements confirm the presence of particulate amines and
its marine-biogenic source at another Arctic site (Alert, 82.5∘ N)
. Future widespread and long-term Arctic measurements of
atmospheric amines would help to extend our results to other regions.
Data can be accessed by contacting the corresponding author F. Köllner (f.koellner@mpic.de).
The Supplement related to this article is available online at https://doi.org/10.5194/acp-17-13747-2017-supplement.
JA, RL and AH
designed the research project. FK, JS, HB, RL, MW and JB carried out the
measurements. AA processed the wind measurements. TK, FH and JS re-designed
and further developed the ALABAMA for aircraft-based measurements. FK
analyzed the data with the help of JS, PH, TK and DK. FK wrote the
manuscript. All co-authors commented on the manuscript.
The authors declare that they have no conflict of
interest.
This article is part of the special issue “NETCARE (Network on
Aerosols and Climate: Addressing Key Uncertainties in Remote Canadian
Environments) (ACP/AMT/BG inter-journal SI)”. It is not associated with a
conference.
Acknowledgements
The authors thank Kenn Borek Air Ltd., in particular our pilots Kevin Elke
and John Bayes, as well as our aircraft maintenance engineer Kevin Riehl. We
thank Jim Hodgson and Lake Central Air Services in Muskoka, Jim Watson (Scale
Modelbuilders, Inc.), Julia Binder and Martin Gehrmann (Alfred Wegener
Institute, AWI) for their support of the integration of the instrumentation
in the aircraft. We thank Bob Christensen (University of Toronto), Lukas Kandora, Manuel Sellmann, Christian Konrad and Jens Herrmann (AWI),
Desiree Toom, Sangeeta Sharma (ECCC), Kathy Law and Jenny Thomas (LATMOS) for their
support before and during the study. We thank Christiane Schulz (MPIC) for
her support during the integration of the instruments in Muskoka. We thank
the Biogeochemistry Department of MPIC for providing the CO instrument and
Dieter Scharffe for his support during the preparation phase of the campaign.
We thank the Nunavut Research Institute and the Nunavut Impact Review Board
for licensing the study. Logistical support in Resolute Bay was provided by
the Polar Continental Shelf Project (PCSP) of Natural Resources Canada under
PCSP field project 218-14. Funding for this work was provided by the Natural
Sciences and Engineering Research Council of Canada through the NETCARE
project of the Climate Change and Atmospheric Research Program, the Alfred
Wegener Institute, Environment and Climate Change Canada and the Max Planck
Society. Special thanks to the whole NETCARE team for data exchange,
discussions and support. The article processing
charges for this open-access publication were covered by the
Max Planck Society.
Edited by: Barbara Ervens
Reviewed by: three anonymous referees
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