Physicochemical properties and origin of organic groups detected in boreal forest using an aerosol mass spectrometer

Abstract. An Aerodyne quadrupole aerosol mass spectrometer (Q-AMS) was deployed in Hyytiälä, a forested rural measurement site in southern Finland, during a 2-week measurement campaign in spring 2005. Q-AMS measures mass concentrations of non-refractory species including sulphate, nitrate, ammonium and organics from submicron particles. A positive matrix factorization method was used in identifying two oxygenated organic aerosol (OOA) groups from the measured total organic mass. The properties of these groups were estimated from their diurnal concentration cycles and correlations with additional data such as air mass history, particle number size distributions, hygroscopic and ethanol growth factors and particle volatility. It was found that the aged and highly oxidized background organic aerosol (OOA1 or LV-OOA) species have a wide range of hygroscopic growth factors and volatilization temperatures, but on the average OOA1 is the less volatile and more hygroscopic organic group. Hygroscopic properties and volatilities of the OOA1 species are correlated so that the less volatile species have higher hygroscopic growth factors. The other, less oxidized organic aerosol group (OOA2 or SV-OOA) is more volatile and non-hygroscopic. Trajectory analysis showed that OOA1 and the inorganic species are mainly long-range transported anthropogenic pollutions. OOA2 species and its precursor gases have short atmospheric life times, so they are from local sources. These results span the range of previous observations of oxygen content, volatility and hygroscopic growth factor, simultaneously coupling all three measurements for the first time.

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Physicochemical properties and origin of organic groups detected in boreal forest using an aerosol mass spectrometer

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-9-21847-2009 ◽

2009 ◽

Vol 9 (5) ◽

pp. 21847-21889 ◽

Cited By ~ 2

Author(s):

T. Raatikainen ◽

P. Vaattovaara ◽

P. Tiitta ◽

P. Miettinen ◽

J. Rautiainen ◽

...

Keyword(s):

Growth Factors ◽

Mass Spectrometer ◽

Additional Data ◽

Organic Aerosol ◽

The Other ◽

Hygroscopic Growth ◽

Aerosol Mass Spectrometer ◽

Aerosol Mass ◽

Hygroscopic Properties ◽

Wide Range

Abstract. An Aerodyne quadrupole aerosol mass spectrometer (Q-AMS) was deployed in Hyytiälä, a forested rural measurement site in southern Finland, during a 2-week measurement campaign in spring 2005. Q-AMS measures mass concentrations of non-refractory species including sulphate, nitrate, ammonium and organics from submicron particles. A positive matrix factorization method was used in identifying two oxygenated organic aerosol (OOA) groups from the measured total organic mass. The properties of these groups were estimated from their diurnal concentration cycles and correlations with additional data such as air mass history, particle number size distributions, hygroscopic and ethanol growth factors and particle volatility. It was found that the aged and highly oxidized background organic aerosol (OOA1) species have a wide range of hygroscopic growth factors and volatilization temperatures, but on the average OOA1 is the less volatile and hygroscopic organic group. It seems that hygroscopic properties and volatilities of the OOA1 species are correlated so that the less volatile species have higher hygroscopic growth factors. The other less oxidized organic aerosol group (OOA2) is more volatile and non-hygroscopic. Trajectory analysis showed that OOA1 and the inorganic species are mainly long-range transported anthropogenic pollutions. On the other hand, OOA2 species and its precursor gases have short atmospheric life times, so they are from local sources. Current results are in good agreement with previous studies, but additional data especially from other seasons is required to verify the generality of the conclusions.

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Formation of secondary organic aerosol coating on black carbon particles near vehicular emissions

10.5194/acp-2017-665 ◽

2017 ◽

Cited By ~ 1

Author(s):

Alex K. Y. Lee ◽

Chia-Li Chen ◽

Jun Liu ◽

Derek J. Price ◽

Raghu Betha ◽

...

Keyword(s):

Black Carbon ◽

Mass Spectrometer ◽

Secondary Organic Aerosol ◽

Spectral Characteristics ◽

Organic Aerosol ◽

Vehicular Emissions ◽

Aerosol Mass Spectrometer ◽

Diurnal Cycles ◽

Aerosol Mass ◽

Inorganic Species

Abstract. Black carbon (BC) emitted from incomplete combustion can result in significant impacts on air quality and climate. Understanding the mixing state of ambient BC and the chemical characteristics of its associated coatings are particularly important to evaluate BC fate and environmental impacts. In this study, we investigate the formation of organic coatings on BC particles in an urban environment (Fontana, California) under hot and dry conditions using a Soot-Particle Aerosol Mass Spectrometer (SP-AMS). The SP-AMS was operated in a configuration that can detect refractory BC (rBC) particles and their coatings exclusively. Using the −log(NOx/NOy) ratio as a proxy for photochemical age of air masses, substantial formation of secondary organic aerosol (SOA) coatings on rBC particles was observed due to active photochemistry in the afternoon, whereas primary organic aerosol (POA) components were strongly associated with rBC from fresh vehicular missions in the morning rush hours. There is also evidence that cooking related organic aerosols were externally mixed from rBC. Positive matrix factorization and elemental analysis illustrate that most of the observed SOA coatings were freshly formed, providing an opportunity to examine SOA coating formation on rBC near vehicular emissions. Approximately 7–20 wt % of secondary organic and inorganic species were estimated to be internally mixed with rBC on average, implying that rBC is unlikely the major condensation sinks of SOA in this study. Diurnal cycles of oxygenated organic aerosol (OOA) observed by a co-located standard high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-MS) correlated well with that of SOA coatings on rBC, but their mass spectral characteristics were different from each other. Our results suggest that at least a portion of SOA materials condensed on rBC surface were chemically different from OOA particles that were externally mixed with rBC, although they are both generated from local photochemistry.

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Factor analysis of combined organic and inorganic aerosol mass spectra from high resolution aerosol mass spectrometer measurements

Atmospheric Chemistry and Physics ◽

10.5194/acp-12-8537-2012 ◽

2012 ◽

Vol 12 (18) ◽

pp. 8537-8551 ◽

Cited By ~ 67

Author(s):

Y. L. Sun ◽

Q. Zhang ◽

J. J. Schwab ◽

T. Yang ◽

N. L. Ng ◽

...

Keyword(s):

High Resolution ◽

Ammonium Nitrate ◽

Mass Spectrometer ◽

Mass Spectra ◽

Organic Aerosol ◽

Organic Nitrates ◽

Spectral Matrix ◽

Aerosol Mass Spectrometer ◽

Aerosol Mass ◽

Inorganic Species

Abstract. Positive matrix factorization (PMF) was applied to the merged high resolution mass spectra of organic and inorganic aerosols from aerosol mass spectrometer (AMS) measurements to investigate the sources and evolution processes of submicron aerosols in New York City in summer 2009. This new approach is able to study the distribution of organic and inorganic species in different types of aerosols, the acidity of organic aerosol (OA) factors, and the fragment ion patterns related to photochemical processing. In this study, PMF analysis of the unified AMS spectral matrix resolved 8 factors. The hydrocarbon-like OA (HOA) and cooking OA (COA) factors contain negligible amounts of inorganic species. The two factors that are primarily ammonium sulfate (SO4-OA) and ammonium nitrate (NO3-OA), respectively, are overall neutralized. Among all OA factors the organic fraction of SO4-OA shows the highest degree of oxidation (O/C = 0.69). Two semi-volatile oxygenated OA (OOA) factors, i.e., a less oxidized (LO-OOA) and a more oxidized (MO-OOA), were also identified. MO-OOA represents local photochemical products with a diurnal profile exhibiting a pronounced noon peak, consistent with those of formaldehyde (HCHO) and Ox(= O3 + NO2). The NO+/NO2+ ion ratio in MO-OOA is much higher than that in NO3-OA and in pure ammonium nitrate, indicating the formation of organic nitrates. The nitrogen-enriched OA (NOA) factor contains ~25% of acidic inorganic salts, suggesting the formation of secondary OA via acid-base reactions of amines. The size distributions of OA factors derived from the size-resolved mass spectra show distinct diurnal evolving behaviors but overall a progressing evolution from smaller to larger particle mode as the oxidation degree of OA increases. Our results demonstrate that PMF analysis of the unified aerosol mass spectral matrix which contains both inorganic and organic aerosol signals may enable the deconvolution of more OA factors and gain more insights into the sources, processes, and chemical characteristics of OA in the atmosphere.

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Formation of secondary organic aerosol coating on black carbon particles near vehicular emissions

Atmospheric Chemistry and Physics ◽

10.5194/acp-17-15055-2017 ◽

2017 ◽

Vol 17 (24) ◽

pp. 15055-15067 ◽

Cited By ~ 14

Author(s):

Alex K. Y. Lee ◽

Chia-Li Chen ◽

Jun Liu ◽

Derek J. Price ◽

Raghu Betha ◽

...

Keyword(s):

Black Carbon ◽

Mass Spectrometer ◽

Secondary Organic Aerosol ◽

Organic Aerosol ◽

Vehicular Emissions ◽

Aerosol Mass Spectrometer ◽

Carbon Particles ◽

Aerosol Mass ◽

Inorganic Species ◽

Dry Conditions

Abstract. Black carbon (BC) emitted from incomplete combustion can result in significant impacts on air quality and climate. Understanding the mixing state of ambient BC and the chemical characteristics of its associated coatings is particularly important to evaluate BC fate and environmental impacts. In this study, we investigate the formation of organic coatings on BC particles in an urban environment (Fontana, California) under hot and dry conditions using a soot-particle aerosol mass spectrometer (SP-AMS). The SP-AMS was operated in a configuration that can exclusively detect refractory BC (rBC) particles and their coatings. Using the −log(NOx ∕ NOy) ratio as a proxy for photochemical age of air masses, substantial formation of secondary organic aerosol (SOA) coatings on rBC particles was observed due to active photochemistry in the afternoon, whereas primary organic aerosol (POA) components were strongly associated with rBC from fresh vehicular emissions in the morning rush hours. There is also evidence that cooking-related organic aerosols were externally mixed from rBC. Positive matrix factorization and elemental analysis illustrate that most of the observed SOA coatings were freshly formed, providing an opportunity to examine SOA coating formation on rBCs near vehicular emissions. Approximately 7–20 wt % of secondary organic and inorganic species were estimated to be internally mixed with rBC on average, implying that rBC is unlikely the major condensation sink of SOA in this study. Comparison of our results to a co-located standard high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) measurement suggests that at least a portion of SOA materials condensed on rBC surfaces were chemically different from oxygenated organic aerosol (OOA) particles that were externally mixed with rBC, although they could both be generated from local photochemistry.

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Reconciliation of measurements of hygroscopic growth and critical supersaturation of aerosol particles in central Germany

Atmospheric Chemistry and Physics ◽

10.5194/acp-10-11737-2010 ◽

2010 ◽

Vol 10 (23) ◽

pp. 11737-11752 ◽

Cited By ~ 45

Author(s):

M. Irwin ◽

N. Good ◽

J. Crosier ◽

T. W. Choularton ◽

G. McFiggans

Keyword(s):

Growth Factors ◽

Water Uptake ◽

Single Parameter ◽

Hygroscopic Growth ◽

Aerosol Composition ◽

Aerosol Mass Spectrometer ◽

Aerosol Mass ◽

Hygroscopic Properties ◽

Critical Supersaturation ◽

Activity Measurements

Abstract. Aerosol physical, chemical and hygroscopic properties were measured in a range of airmasses during COPS (Convective and Orographically-induced Precipitation Study) ground-based in June and July of 2007 at the Hornisgrinde mountain site in the Black Forest, Southwest Germany. Non-refractory aerosol composition was measured with an Aerosol Mass Spectrometer, simultaneous to hygroscopic growth factors at 86% relative humidity and CCN activity measurements for particles of dry (<20%) diameters 27 to 217 nm, with particle water uptake exhibiting substantial variability with time and with particle size. Variability in the measurements of hygroscopic growth factor and critical supersaturation for particles of similar sizes indicates significant compositional impact on particle water affinity. Critical supersaturation prediction using a single parameter hygroscopicity approximation derived from measured HTDMA mean growth factors deviate, beyond measurement uncertainties, from critical supersaturations derived from CCN measurements. These led to differences averaging around 35% in the number of CCN (NCCN) for the most reliable measurements depending on averaging methodology, often very much larger for individual time periods. This indicates aspects of water uptake behaviour unresolved in this experiment by the single parameter representation which, depending on its origin, may have important consequences on its generalised use.

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The effect of photochemical ageing and initial precursor concentration on the composition and hygroscopic properties of β-caryophyllene secondary organic aerosol

Atmospheric Chemistry and Physics ◽

10.5194/acp-12-6417-2012 ◽

2012 ◽

Vol 12 (14) ◽

pp. 6417-6436 ◽

Cited By ~ 45

Author(s):

M. R. Alfarra ◽

J. F. Hamilton ◽

K. P. Wyche ◽

N. Good ◽

M. W. Ward ◽

...

Keyword(s):

Mass Spectrometer ◽

Secondary Organic Aerosol ◽

Organic Aerosol ◽

Precursor Concentration ◽

Temporal Behaviour ◽

Elemental Ratios ◽

Aerosol Mass Spectrometer ◽

Initial Concentration ◽

Aerosol Mass ◽

Hygroscopic Properties

Abstract. The effect of photochemical ageing and initial precursor concentration on the composition and hygroscopic properties of secondary organic aerosol (SOA) formed during the chamber photo-oxidation of β-caryophyllene/NOx mixtures were investigated. Nucleation of β-caryophyllene SOA particles occurred almost immediately after oxidation was initiated and led to the formation of fresh SOA with a relatively simpler composition than has been reported for monoterpenes. The SOA yield values ranged from 9.5–26.7% and 30.4–44.5% using a differential mobility particle sizer (DMPS) and an aerosol mass spectrometer (AMS) mass based measurements, respectively. A total of 20 compounds were identified in the SOA by LC-MS/MS, with the most abundant compounds identified as β-caryophyllonic acid and β-caryophyllinic acid/β-nocaryophyllonic acid. The O:C and H:C elemental ratios of products identified in the condensed phase ranged from 0.20 to 1.00 and 1.00 to 2.00, with average values of 0.39 and 1.58, respectively. The increase in the O:C ratio was associated with a decrease in the saturation concentration of the identified compounds. The compounds identified in the lower initial concentration experiments were more oxidised compared to those that were found to be more abundant in the higher initial concentration experiments with average O:C ratios of 0.51 and 0.27, respectively. Photochemical ageing led to a more complex SOA composition with a larger contribution coming from lower molar mass, higher generation products, where both double bonds had been oxidised. This effect was more evident in the experiments conducted using the lower initial precursor concentration; a finding confirmed by the temporal behaviour of key organic mass fragment measured by an Aerosol Mass Spectrometer. Although the composition changed with both initial precursor concentration and ageing, this had no significant measurable effect on the hygroscopic properties of the SOA formed. The latter finding might have been influenced by the difference in pre-treatment of the semivolatile-containing particles prior to their measurements.

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Secondary organic aerosol formation from reaction of tertiary amines with nitrate radical

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-8-16585-2008 ◽

2008 ◽

Vol 8 (4) ◽

pp. 16585-16608 ◽

Cited By ~ 6

Author(s):

M. E. Erupe ◽

D. J. Price ◽

P. J. Silva ◽

Q. G. J. Malloy ◽

L. Qi ◽

...

Keyword(s):

Mass Spectrometer ◽

Secondary Organic Aerosol ◽

Organic Aerosol ◽

Nitrate Radical ◽

Tertiary Amines ◽

Aerosol Formation ◽

Night Time ◽

Aerosol Mass Spectrometer ◽

Aerosol Mass ◽

Secondary Organic Aerosol Formation

Abstract. Secondary organic aerosol formation from the reaction of tertiary amines with nitrate radical was investigated in an indoor environmental chamber. Particle chemistry was monitored using a high resolution aerosol mass spectrometer while gas-phase species were detected using a proton transfer reaction mass spectrometer. Trimethylamine, triethylamine and tributylamine were studied. Results indicate that tributylamine forms the most aerosol mass followed by trimethylamine and triethylamine respectively. Spectra from the aerosol mass spectrometer indicate the formation of complex non-salt aerosol products. We propose a reaction mechanism that proceeds via abstraction of a proton by nitrate radical followed by RO2 chemistry. Rearrangement of the aminyl alkoxy radical through hydrogen shift leads to the formation of hydroxylated amides, which explain most of the higher mass ions in the mass spectra. These experiments show that oxidation of tertiary amines by nitrate radical may be an important night-time source of secondary organic aerosol.

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Characterization of a real-time tracer for isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) from aerosol mass spectrometer measurements

Atmospheric Chemistry and Physics ◽

10.5194/acp-15-11807-2015 ◽

2015 ◽

Vol 15 (20) ◽

pp. 11807-11833 ◽

Cited By ~ 121

Author(s):

W. W. Hu ◽

P. Campuzano-Jost ◽

B. B. Palm ◽

D. A. Day ◽

A. M. Ortega ◽

...

Keyword(s):

Mass Spectrometer ◽

Secondary Organic Aerosol ◽

Transport Model ◽

Organic Aerosol ◽

Oxidation Products ◽

Chemical Transport Model ◽

Aerosol Mass Spectrometer ◽

Aerosol Mass ◽

Multiple Field

Abstract. Substantial amounts of secondary organic aerosol (SOA) can be formed from isoprene epoxydiols (IEPOX), which are oxidation products of isoprene mainly under low-NO conditions. Total IEPOX-SOA, which may include SOA formed from other parallel isoprene oxidation pathways, was quantified by applying positive matrix factorization (PMF) to aerosol mass spectrometer (AMS) measurements. The IEPOX-SOA fractions of organic aerosol (OA) in multiple field studies across several continents are summarized here and show consistent patterns with the concentration of gas-phase IEPOX simulated by the GEOS-Chem chemical transport model. During the Southern Oxidant and Aerosol Study (SOAS), 78 % of PMF-resolved IEPOX-SOA is accounted by the measured IEPOX-SOA molecular tracers (2-methyltetrols, C5-Triols, and IEPOX-derived organosulfate and its dimers), making it the highest level of molecular identification of an ambient SOA component to our knowledge. An enhanced signal at C5H6O+ (m/z 82) is found in PMF-resolved IEPOX-SOA spectra. To investigate the suitability of this ion as a tracer for IEPOX-SOA, we examine fC5H6O (fC5H6O= C5H6O+/OA) across multiple field, chamber, and source data sets. A background of ~ 1.7 ± 0.1 ‰ (‰ = parts per thousand) is observed in studies strongly influenced by urban, biomass-burning, and other anthropogenic primary organic aerosol (POA). Higher background values of 3.1 ± 0.6 ‰ are found in studies strongly influenced by monoterpene emissions. The average laboratory monoterpene SOA value (5.5 ± 2.0 ‰) is 4 times lower than the average for IEPOX-SOA (22 ± 7 ‰), which leaves some room to separate both contributions to OA. Locations strongly influenced by isoprene emissions under low-NO levels had higher fC5H6O (~ 6.5 ± 2.2 ‰ on average) than other sites, consistent with the expected IEPOX-SOA formation in those studies. fC5H6O in IEPOX-SOA is always elevated (12–40 ‰) but varies substantially between locations, which is shown to reflect large variations in its detailed molecular composition. The low fC5H6O (< 3 ‰) reported in non-IEPOX-derived isoprene-SOA from chamber studies indicates that this tracer ion is specifically enhanced from IEPOX-SOA, and is not a tracer for all SOA from isoprene. We introduce a graphical diagnostic to study the presence and aging of IEPOX-SOA as a triangle plot of fCO2 vs. fC5H6O. Finally, we develop a simplified method to estimate ambient IEPOX-SOA mass concentrations, which is shown to perform well compared to the full PMF method. The uncertainty of the tracer method is up to a factor of ~ 2, if the fC5H6O of the local IEPOX-SOA is not available. When only unit mass-resolution data are available, as with the aerosol chemical speciation monitor (ACSM), all methods may perform less well because of increased interferences from other ions at m/z 82. This study clarifies the strengths and limitations of the different AMS methods for detection of IEPOX-SOA and will enable improved characterization of this OA component.

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Collection efficiency of the soot-particle aerosol mass spectrometer (SP-AMS) for internally mixed particulate black carbon

Atmospheric Measurement Techniques ◽

10.5194/amt-7-4507-2014 ◽

2014 ◽

Vol 7 (12) ◽

pp. 4507-4516 ◽

Cited By ~ 44

Author(s):

M. D. Willis ◽

A. K. Y. Lee ◽

T. B. Onasch ◽

E. C. Fortner ◽

L. R. Williams ◽

...

Keyword(s):

Laser Beam ◽

Black Carbon ◽

Mass Spectrometer ◽

Soot Particle ◽

Collection Efficiency ◽

Particle Beam ◽

Aerosol Mass Spectrometer ◽

Coated Particles ◽

Aerosol Mass ◽

Wide Range

Abstract. The soot-particle aerosol mass spectrometer (SP-AMS) uses an intra-cavity infrared laser to vaporize refractory black carbon (rBC) containing particles, making the particle beam–laser beam overlap critical in determining the collection efficiency (CE) for rBC and associated non-refractory particulate matter (NR-PM). This work evaluates the ability of the SP-AMS to quantify rBC and NR-PM mass in internally mixed particles with different thicknesses of organic coating. Using apparent relative ionization efficiencies for uncoated and thickly coated rBC particles, we report measurements of SP-AMS sensitivity to NR-PM and rBC, for Regal Black, the recommended particulate calibration material. Beam width probe (BWP) measurements are used to illustrate an increase in sensitivity for highly coated particles due to narrowing of the particle beam, which enhances the CE of the SP-AMS by increasing the laser beam–particle beam overlap. Assuming complete overlap for thick coatings, we estimate CE for bare Regal Black particles of 0.6 ± 0.1, which suggests that previously measured SP-AMS sensitivities to Regal Black were underestimated by up to a factor of 2. The efficacy of the BWP measurements is highlighted by studies at a busy road in downtown Toronto and at a non-roadside location, which show particle beam widths similar to, but greater than that of bare Regal Black and coated Regal Black, respectively. Further BWP measurements at field locations will help to constrain the range of CE for fresh and aged rBC-containing particles. The ability of the SP-AMS to quantitatively assess the composition of internally mixed particles is validated through measurements of laboratory-generated organic coated particles, which demonstrate that the SP-AMS can quantify rBC and NR-PM over a wide range of particle compositions and rBC core sizes.

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The real part of the refractive indices and effective densities for chemically segregated ambient aerosols in Guangzhou measured by a single-particle aerosol mass spectrometer

Atmospheric Chemistry and Physics ◽

10.5194/acp-16-2631-2016 ◽

2016 ◽

Vol 16 (4) ◽

pp. 2631-2640 ◽

Cited By ~ 6

Author(s):

Guohua Zhang ◽

Xinhui Bi ◽

Ning Qiu ◽

Bingxue Han ◽

Qinhao Lin ◽

...

Keyword(s):

Mass Spectrometer ◽

Atmospheric Aerosols ◽

Single Particle ◽

Refractive Indices ◽

Chemical Compositions ◽

Aerosol Mass Spectrometer ◽

The Real ◽

Aerosol Mass ◽

Wide Range ◽

The Impact

Abstract. Knowledge on the microphysical properties of atmospheric aerosols is essential to better evaluate their radiative forcing. This paper presents an estimate of the real part of the refractive indices (n) and effective densities (ρeff) of chemically segregated atmospheric aerosols in Guangzhou, China. Vacuum aerodynamic diameter, chemical compositions, and light-scattering intensities of individual particles were simultaneously measured by a single-particle aerosol mass spectrometer (SPAMS) during the fall of 2012. On the basis of Mie theory, n at a wavelength of 532 nm and ρeff were estimated for 17 particle types in four categories: organics (OC), elemental carbon (EC), internally mixed EC and OC (ECOC), and Metal-rich. The results indicate the presence of spherical or nearly spherical shapes for the majority of particle types, whose partial scattering cross-section versus sizes were well fitted to Mie theoretical modeling results. While sharing n in a narrow range (1.47–1.53), majority of particle types exhibited a wide range of ρeff (0.87–1.51 g cm−3). The OC group is associated with the lowest ρeff (0.87–1.07 g cm−3), and the Metal-rich group with the highest ones (1.29–1.51 g cm−3). It is noteworthy that a specific EC type exhibits a complex scattering curve versus size due to the presence of both compact and irregularly shaped particles. Overall, the results on the detailed relationship between physical and chemical properties benefits future research on the impact of aerosols on visibility and climate.

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