scholarly journals Application of positive matrix factor analysis in heterogeneous kinetics studies: an improvement to the mixed-phase relative rates technique

2014 ◽  
Vol 14 (6) ◽  
pp. 8695-8722 ◽  
Author(s):  
Y. Liu ◽  
S.-M. Li ◽  
J. Liggio
Keyword(s):  
Citric Acid ◽  
Heterogeneous Reaction ◽  
Organic Aerosol ◽  
Mixed Phase ◽  
Oxidation Products ◽  
Oh Radicals ◽  
Positive Matrix ◽  
Heterogeneous Kinetics ◽  
Aerosol Mass ◽  
Uptake Coefficients

Abstract. The mixed-phase relative rate approach for determining aerosol particle organic component heterogeneous reaction kinetics and OH uptake coefficients to particles is often performed utilizing mass spectral tracers as a proxy for particle phase reactant concentration. However, this approach may be influenced by signal contaminations from oxidation products during the experiment. In the current study, the mixed-phase relative rates technique has been improved by combining a Positive Matrix Factor (PMF) analysis with electron ionization Aerosol Mass Spectrometry, thereby removing the influence of m / z fragments from reaction products on the reactant signals. To demonstrate the advantages of this approach, the heterogeneous reaction between OH radicals and citric acid (CA) was investigated using a photochemical flow tube coupled to a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS). The measured heterogeneous rate constant (k2) of citric acid toward OH was (3.31 ± 0.29) × 10−12 cm3 molecule−1 s−1 at 298 K and (30 ± 3)% RH and was ∼7.7 times greater than previously reported results utilizing individual m / z fragments. This phenomenon was further confirmed for particulate-phase organophosphates (TPhP, TDCPP, and TEHP), leading to k2 values significantly larger than previously reported. The results suggest that heterogeneous kinetics can be significantly underestimated when a non-molecular ion peak is used as the tracer. Finally, the results suggest that the heterogeneous lifetime of organic aerosol in models can be overestimated due to underestimated OH uptake coefficients, and that it may be necessary to revisit the heterogeneous kinetic data of organic aerosol components which were derived in the context of the relative rates technique.

scholarly journals Technical Note: Application of positive matrix factor analysis in heterogeneous kinetics studies utilizing the mixed-phase relative rates technique

2014 ◽  
Vol 14 (17) ◽  
pp. 9201-9211 ◽  
Author(s):  
Y. Liu ◽  
S.-M. Li ◽  
J. Liggio
Keyword(s):  
Citric Acid ◽  
Mass Spectrometer ◽  
Rate Constant ◽  
Heterogeneous Reaction ◽  
Mixed Phase ◽  
Positive Matrix ◽  
Aerosol Mass Spectrometer ◽  
Heterogeneous Kinetics ◽  
Aerosol Mass ◽  
Unit Mass Resolution

Abstract. The mixed-phase relative rates approach for determining aerosol particle organic heterogeneous reaction kinetics is often performed utilizing mass spectral tracers as a proxy for particle-phase reactant concentration. However, this approach may be influenced by signal contamination from oxidation products during the experiment. In the current study, the mixed-phase relative rates technique has been improved by combining a positive matrix factor (PMF) analysis with electron ionization aerosol mass spectrometry (unit-mass resolution), thereby removing the influence of m / z fragments from reaction products on the reactant signals. To demonstrate the advantages of this approach, the heterogeneous reaction between OH radicals and citric acid (CA) was investigated using a photochemical flow tube coupled to a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS). The measured heterogeneous rate constant (k2) of citric acid toward OH was (3.31 ± 0.29) × 10−12 cm3 molecule−1 s−1 at 298 K and (30 ± 3)% relative humidity (RH) and was several times greater than the results utilizing individual m / z fragments. This phenomenon was further evaluated for particulate-phase organophosphates (triphenyl phosphate (TPhP), tris-1,3-dichloro-2-propyl phosphate (TDCPP) and tris-2-ethylhexyl phosphate (TEHP)), leading to k2 values significantly larger than previously reported. The results suggest that heterogeneous kinetics can be significantly underestimated when the structure of the products is highly similar to the reactant and when a non-molecular tracer is measured with a unit-mass resolution aerosol mass spectrometer. The results also suggest that the heterogeneous lifetime of organic aerosol in models can be overestimated due to underestimated OH uptake coefficients. Finally, a comparison of reported rate constants implies that the heterogeneous oxidation of aerosols will be dependent upon a number of factors related to the reaction system, and that a single rate constant for one system cannot be universally applied under all conditions.

scholarly journals Development of a versatile source apportionment analysis based on positive matrix factorization: a case study of the seasonal variation of organic aerosol sources in Estonia

2019 ◽  
Vol 19 (11) ◽  
pp. 7279-7295 ◽  
Author(s):  
Athanasia Vlachou ◽  
Anna Tobler ◽  
Houssni Lamkaddam ◽  
Francesco Canonaco ◽  
Kaspar R. Daellenbach ◽  
...  
Keyword(s):  
Matrix Factorization ◽  
Organic Aerosol ◽  
Positive Matrix Factorization ◽  
Water Soluble ◽  
Oxidation Products ◽  
Positive Matrix ◽  
Bootstrap Analysis ◽  
Seasonal Behavior ◽  
Yearly Cycle ◽  
Aerosol Mass

Abstract. Bootstrap analysis is commonly used to capture the uncertainties of a bilinear receptor model such as the positive matrix factorization (PMF) model. This approach can estimate the factor-related uncertainties and partially assess the rotational ambiguity of the model. The selection of the environmentally plausible solutions, though, can be challenging, and a systematic approach to identify and sort the factors is needed. For this, comparison of the factors between each bootstrap run and the initial PMF output, as well as with externally determined markers, is crucial. As a result, certain solutions that exhibit suboptimal factor separation should be discarded. The retained solutions would then be used to test the robustness of the PMF output. Meanwhile, analysis of filter samples with the Aerodyne aerosol mass spectrometer and the application of PMF and bootstrap analysis on the bulk water-soluble organic aerosol mass spectra have provided insight into the source identification and their uncertainties. Here, we investigated a full yearly cycle of the sources of organic aerosol (OA) at three sites in Estonia: Tallinn (urban), Tartu (suburban) and Kohtla-Järve (KJ; industrial). We identified six OA sources and an inorganic dust factor. The primary OA types included biomass burning, dominant in winter in Tartu and accounting for 73 % ± 21 % of the total OA, primary biological OA which was abundant in Tartu and Tallinn in spring (21 % ± 8 % and 11 % ± 5 %, respectively), and two other primary OA types lower in mass. A sulfur-containing OA was related to road dust and tire abrasion which exhibited a rather stable yearly cycle, and an oil OA was connected to the oil shale industries in KJ prevailing at this site that comprises 36 % ± 14 % of the total OA in spring. The secondary OA sources were separated based on their seasonal behavior: a winter oxygenated OA dominated in winter (36 % ± 14 % for KJ, 25 % ± 9 % for Tallinn and 13 % ± 5 % for Tartu) and was correlated with benzoic and phthalic acid, implying an anthropogenic origin. A summer oxygenated OA was the main source of OA in summer at all sites (26 % ± 5 % in KJ, 41 % ± 7 % in Tallinn and 35 % ± 7 % in Tartu) and exhibited high correlations with oxidation products of a-pinene-like pinic acid and 3-methyl-1, 2, 3-butanetricarboxylic acid (MBTCA), suggesting a biogenic origin.

scholarly journals Chemical evolution of secondary organic aerosol from OH-initiated heterogeneous oxidation

2010 ◽  
Vol 10 (2) ◽  
pp. 3265-3300 ◽  
Author(s):  
I. J. George ◽  
J. P. D. Abbatt
Keyword(s):  
Mass Spectra ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Oxidation Products ◽  
Oh Radicals ◽  
Heterogeneous Oxidation ◽  
Atmospheric Aging ◽  
Aerosol Mass ◽  
Degree Of Oxidation ◽  
Aerosol Aging

Abstract. The heterogeneous oxidation of laboratory Secondary Organic Aerosol (SOA) particles by OH radicals was investigated. SOA particles, produced by reaction of α-pinene and O3, were exposed to OH radicals in a flow tube, and particle chemical composition, size, and hygroscopicity were measured to assess modifications due to oxidative aging. Aerosol Mass Spectrometer (AMS) mass spectra indicated that the degree of oxidation of SOA particles was significantly enhanced due to OH-initiated oxidation. Particle O/C ratios calculated from m/z 44 fraction from organic mass spectra rose by a maximum of ~0.04 units under equivalent atmospheric aging timescales of 2 weeks assuming a 24-h average OH concentration of 106 cm−3. Particle densities also increased with heterogeneous oxidation, consistent with the observed increase in the degree of oxidation. Minor reductions in particle size, with volume losses of up to 10%, were observed due to volatilization of oxidation products. The SOA particles became slightly more CCN active with an increase in the κ hygroscopicity parameter of up to a factor of two for the equivalent of 2 weeks of OH atmospheric exposure. These results indicate that OH heterogeneous oxidation of typical SOA proceeds sufficiently rapidly to be an atmospherically important organic aerosol aging mechanism.

scholarly journals Development of a versatile source apportionment analysis based on positive matrix factorization: a case study of the seasonal variation of organic aerosol sources in Estonia

2018 ◽  
Author(s):  
Athanasia Vlachou ◽  
Anna Tobler ◽  
Houssni Lamkaddam ◽  
Francesco Canonaco ◽  
Kaspar R. Daellenbach ◽  
...  
Keyword(s):  
Road Dust ◽  
Organic Aerosol ◽  
Bulk Water ◽  
Water Soluble ◽  
Oxidation Products ◽  
Positive Matrix ◽  
Bootstrap Analysis ◽  
Yearly Cycle ◽  
Pmf Model ◽  
Aerosol Mass

Abstract. Bootstrap analysis is commonly used to capture the uncertainties of a bilinear receptor model such as the positive matrix factorisation (PMF) model. This approach can estimate the factor related uncertainties and partially assess the rotational ambiguity of the model. The selection of the environmentally plausible solutions though can be challenging and a systematic approach to identify and sort the factors is needed. For this, comparison of the factors between each bootstrap run and the initial PMF output, as well as with externally determined markers, is crucial. As a result, certain solutions that exhibit sub-optimal factor separation should be discarded. The retained solutions would then be used to test the robustness of the PMF output. Meanwhile, analysis of filter sample with the Aerodyne aerosol mass spectrometer and the application of PMF and bootstrap analysis on the bulk water soluble organic aerosol mass spectra has provided insight into the source identification and their uncertainties. Here, we investigated a full yearly cycle of the sources of organic aerosol (OA) at three sites in Estonia, Tallinn (urban), Tartu (suburban) and Kohtla–Järve (KJ, industrial). We identified six OA sources and an inorganic dust factor. The primary OA types included biomass burning, dominant in winter in Tartu accounting for 73 % ± 21 % of the total OA, primary biological OA which was abundant in Tartu and Tallinn in spring (21 % ± 8 % and 11 % ± 5 %, respectively) and two other primary OA types lower in mass. A sulphur containing OA was related to road dust and tire abrasion which exhibited a rather stable yearly cycle and an oil OA was connected to the oil shale industries in KJ prevailing at this site comprising 36 % ± 14 % of the total OA in spring. The secondary OA sources were separated based on their seasonal behaviour: a winter oxygenated OA dominated in winter (36 % ± 14 % for KJ, 25 % ± 9 % for Tallinn and 13 % ± 5 % for Tartu) and was correlated with benzoic and phthalic acid implying an anthropogenic origin. A summer oxygenated OA was the main source of OA in summer at all sites (26 % ± 5 % in KJ, 41 % ± 7 % in Tallinn and 35 % ± 7 % in Tartu) and exhibited high correlations with oxidation products of α-pinene like pinic acid and 3-methyl-1, 2, 3-butanetricarboxylic acid (MBTCA) suggesting a biogenic origin.

scholarly journals Chemical evolution of secondary organic aerosol from OH-initiated heterogeneous oxidation

2010 ◽  
Vol 10 (12) ◽  
pp. 5551-5563 ◽  
Author(s):  
I. J. George ◽  
J. P. D. Abbatt
Keyword(s):  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Oxidation Products ◽  
Oh Radicals ◽  
Cloud Droplets ◽  
Heterogeneous Oxidation ◽  
Atmospheric Aging ◽  
Aerosol Mass ◽  
Degree Of Oxidation ◽  
Aging Mechanisms

Abstract. The heterogeneous oxidation of laboratory Secondary Organic Aerosol (SOA) particles by OH radicals was investigated. SOA particles, produced by reaction of α-pinene and O3, were exposed to OH radicals in a flow tube, and particle chemical composition, size, and hygroscopicity were measured to assess modifications due to oxidative aging. Aerosol Mass Spectrometer (AMS) mass spectra indicated that the degree of oxidation of 200 nm diameter SOA particles was significantly enhanced due to OH-initiated oxidation, as evidenced by the increase in the fraction of m/z 44 fragment of total organic mass concentration (F44). F44 values of the SOA particles, initially in the range F44=0.04–0.07, increased by up to ΔF44~0.01 under equivalent atmospheric aging timescales of 2 weeks, assuming a 24-h average OH concentration of 106 cm−3. Particle O/C ratios calculated from F44 values, initially in the range O/C=0.25–0.35, rose by a maximum of ΔO/C~0.04 units for 2 weeks of aging. Particle densities also increased with heterogeneous oxidation, consistent with the observed increase in the degree of oxidation. Minor reductions in particle size, with volume losses of up to 10%, were observed due to volatilization of oxidation products. The SOA particles activated more readily to form cloud droplets with an increase in the κ hygroscopicity parameter of up to a factor of two for the equivalent of 2 weeks of OH atmospheric exposure. These results indicate that OH heterogeneous oxidation of typical SOA needs to be considered as an atmospheric organic aerosol aging mechanism, most likely of higher relative importance away from VOC source regions, where other aging mechanisms are less dominant.

scholarly journals Secondary organic aerosol formation from biomass burning emissions

2019 ◽  
Author(s):  
Christopher Y. Lim ◽  
David H. Hagan ◽  
Matthew M. Coggon ◽  
Abigail R. Koss ◽  
Kanako Sekimoto ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Secondary Organic Aerosol ◽  
Total Concentration ◽  
Organic Aerosol ◽  
Oh Radicals ◽  
Aerosol Formation ◽  
Atmospheric Aging ◽  
Aerosol Mass ◽  
Photochemical Aging ◽  
Organic Gases

Abstract. Biomass burning is an important source of aerosol and trace gases to the atmosphere, but how these emissions change chemically during their lifetimes is not fully understood. As part of the Fire Influence on Regional and Global Environments Experiment (FIREX 2016), we investigated the effect of photochemical aging on biomass burning organic aerosol (BBOA), with a focus on fuels from the western United States. Emissions were sampled into a small (150 L) environmental chamber and photochemically aged via the addition of ozone and irradiation by 254 nm light. While some fraction of species undergoes photolysis, the vast majority of aging occurs via reaction with OH radicals, with total OH exposures corresponding to the equivalent of up to 10 days of atmospheric oxidation. For all fuels burned, large and rapid changes are seen in the ensemble chemical composition of BBOA, as measured by an aerosol mass spectrometer (AMS). Secondary organic aerosol (SOA) formation is seen for all aging experiments and continues to grow with increasing OH exposure, but the magnitude of the SOA formation is highly variable between experiments. This variability can be explained well by a combination of experiment-to-experiment differences in OH exposure and the total concentration of non-methane organic gases (NMOGs) in the chamber before oxidation, measured by PTR-ToF-MS (r2 values from 0.64 to 0.83). From this relationship, we calculate the fraction of carbon from biomass burning NMOGs that is converted to SOA as a function of equivalent atmospheric aging time, with carbon yields ranging from 24 ± 4 % after 6 hours to 56 ± 9 % after 4 days.

scholarly journals Large contribution to secondary organic aerosol from isoprene cloud chemistry

2021 ◽  
Vol 7 (13) ◽  
pp. eabe2952
Author(s):  
Houssni Lamkaddam ◽  
Josef Dommen ◽  
Ananth Ranjithkumar ◽  
Hamish Gordon ◽  
Günther Wehrle ◽  
...  
Keyword(s):  
Radiative Forcing ◽  
Flow Reactor ◽  
Secondary Organic Aerosol ◽  
Cloud Droplet ◽  
Organic Aerosol ◽  
Global Scale ◽  
Oxidation Products ◽  
Oh Radicals ◽  
Large Contribution ◽  
Cloud Processing

Aerosols still present the largest uncertainty in estimating anthropogenic radiative forcing. Cloud processing is potentially important for secondary organic aerosol (SOA) formation, a major aerosol component: however, laboratory experiments fail to mimic this process under atmospherically relevant conditions. We developed a wetted-wall flow reactor to simulate aqueous-phase processing of isoprene oxidation products (iOP) in cloud droplets. We find that 50 to 70% (in moles) of iOP partition into the aqueous cloud phase, where they rapidly react with OH radicals, producing SOA with a molar yield of 0.45 after cloud droplet evaporation. Integrating our experimental results into a global model, we show that clouds effectively boost the amount of SOA. We conclude that, on a global scale, cloud processing of iOP produces 6.9 Tg of SOA per year or approximately 20% of the total biogenic SOA burden and is the main source of SOA in the mid-troposphere (4 to 6 km).

Investigating the NO-dependent photooxidation of limonene by OH and O3 using the atmosphere simulation chamber SAPHIR

2021 ◽  
Author(s):  
Yat Sing Pang ◽  
Martin Kaminski ◽  
Anna Novelli ◽  
Philip Carlsson ◽  
Ismail-Hakki Acir ◽  
...  
Keyword(s):  
Organic Aerosol ◽  
Oxidation Products ◽  
Chemical Mechanism ◽  
Reaction Pathways ◽  
Oh Radicals ◽  
Oh Radical ◽  
Simulation Experiments ◽  
Master Chemical Mechanism ◽  
Simulation Results ◽  
Atmosphere Simulation Chamber

<p>Limonene is the fourth-most abundant monoterpene in the atmosphere, which upon oxidation leads to the formation of secondary organic aerosol (SOA) and thereby influences climate and air quality.</p><p>In this study, the oxidation of limonene by OH at different atmospherically relevant NO and HO<sub>2</sub> levels (NO: 0.1 – 10 ppb; HO<sub>2</sub>: 20 ppt) was investigated in simulation experiments in the SAPHIR chamber at Forschungszentrum Jülich. The analysis focuses on comparing measured radical concentrations (RO<sub>2</sub>, HO<sub>2</sub>, OH) and OH reactivity (k<sub>OH</sub>) with modeled values calculated using the Master Chemical Mechanism (MCM) version 3.3.1.</p><p>At high and medium NO concentrations, RO<sub>2</sub> is expected to quickly react with NO. An HO<sub>2</sub> radical is produced during the process that can be converted back to an OH radical by another reaction with NO. Consistently, for experiments conducted at medium NO levels (~0.5 ppb, RO<sub>2</sub> lifetime ~10 s), simulated RO<sub>2</sub>, HO<sub>2</sub>, and OH agree with observations within the measurement uncertainties, if the OH reactivity of oxidation products is correctly described.</p><p>At lower NO concentrations, the regeneration of HO<sub>2</sub> in the RO<sub>2</sub> + NO reaction is slow and the reaction of RO<sub>2</sub> with HO<sub>2</sub> gains importance in forming peroxides. However, simulation results show a large discrepancy between calculated radical concentrations and measurements at low NO levels (<0.1 ppb, RO<sub>2</sub> lifetime ~ 100 s). Simulated RO<sub>2</sub> concentrations are found to be overestimated by a factor of three; simulated HO<sub>2</sub> concentrations are underestimated by 50 %; simulated OH concentrations are underestimated by about 35%, even if k<sub>OH</sub> is correctly described. This suggests that there could be additional RO<sub>2</sub> reaction pathways that regenerate HO<sub>2</sub> and OH radicals become important, but they are not taken into account in the MCM model.</p>

scholarly journals Volatility and hygroscopicity of aging secondary organic aerosol in a smog chamber

2011 ◽  
Vol 11 (3) ◽  
pp. 7423-7467 ◽  
Author(s):  
T. Tritscher ◽  
J. Dommen ◽  
P. F. DeCarlo ◽  
P. B. Barmet ◽  
A. P. Praplan ◽  
...  
Keyword(s):  
Volume Fraction ◽  
Organic Aerosol ◽  
Heterogeneous Reactions ◽  
Physical Parameters ◽  
Oh Radicals ◽  
Smog Chamber ◽  
Chemical Aging ◽  
Aerosol Mass ◽  
Gas Phase Oxidation ◽  
Substantial Change

Abstract. The evolution of secondary organic aerosols (SOA) during (photo-)chemical aging processes was investigated in a smog chamber. SOA from 10–40 ppb α-pinene was formed during ozonolysis followed by aging with OH radicals. The particles' volatility and hygroscopicity (expressed as volume fraction remaining (VFR) and hygroscopicity parameter κ) were measured with a volatility and hygroscopicity tandem differential mobility analyzer (V/H-TDMA). These measurements were used as sensitive physical parameters to reveal the possible mechanisms responsible for the chemical changes in the SOA composition during aging: A change of VFR and/or κ during processing of atmospheric aerosol may occur either by addition of SOA mass (by condensation) or by an exchange of molecules in the SOA by other molecules with different properties. The former process increases the SOA mass by definition, while the latter keeps the SOA mass roughly constant and may occur either by heterogeneous reactions on the surface of the SOA particles, by homogeneous reactions like oligomerization or by an evaporation – gas-phase oxidation – recondensation cycle. Thus, when there is a substantial change in the aerosol mass with time, the condensation mechanism may be assumed to be dominant, while, when the mass stays roughly constant the exchange mechanism is likely to be dominant, a process termed ripening here. Depending on the phase of the experiment, an O3 mediated condensation, O3 mediated ripening, OH mediated condensation, and OH mediated ripening could be distinguished. During the O3 mediated condensation the particles volatility decreased (increasing VFR) while the hygroscopicity increased. Thereafter, in the course of O3 mediated ripening volatility continued to decrease, but hygroscopicity stayed roughly constant. After exposing the SOA to OH radicals an OH mediated condensation started with a significant increase of SOA mass. Concurrently, hygroscopicity and volatility increased. This phase was then followed by an OH mediated ripening with a decrease of volatility.

scholarly journals In situ secondary organic aerosol formation from ambient pine forest air using an oxidation flow reactor

2015 ◽  
Vol 15 (21) ◽  
pp. 30409-30471 ◽  
Author(s):  
B. B. Palm ◽  
P. Campuzano-Jost ◽  
A. M. Ortega ◽  
D. A. Day ◽  
L. Kaser ◽  
...  
Keyword(s):  
Organic Compounds ◽  
Flow Reactor ◽  
Secondary Organic Aerosol ◽  
Ambient Air ◽  
Organic Aerosol ◽  
Pine Forest ◽  
Oxidation Products ◽  
Oh Radicals ◽  
Aerosol Formation ◽  
Photochemical Aging

Abstract. Ambient air was oxidized by OH radicals in an oxidation flow reactor (OFR) located in a montane pine forest during the BEACHON-RoMBAS campaign to study biogenic secondary organic aerosol (SOA) formation and aging. High OH concentrations and short residence times allowed for semi-continuous cycling through a large range of OH exposures ranging from hours to weeks of equivalent (eq.) atmospheric aging. A simple model is derived and used to account for the relative time scales of condensation of low volatility organic compounds (LVOCs) onto particles, condensational loss to the walls, and further reaction to produce volatile, non-condensing fragmentation products. More SOA production was observed in the OFR at nighttime (average 4 μg m-3 when LVOC fate corrected) compared to daytime (average 1 μg m-3 when LVOC fate corrected), with maximum formation observed at 0.4–1.5 eq. days of photochemical aging. SOA formation followed a similar diurnal pattern to monoterpenes, sesquiterpenes, and toluene + p-cymene concentrations, including a substantial increase just after sunrise at 07:00 LT. Higher photochemical aging (> 10 eq. days) led to a decrease in new SOA formation and a loss of preexisting OA due to heterogeneous oxidation followed by fragmentation and volatilization. When comparing two different commonly used methods of OH production in OFRs (OFR185 and OFR254), similar amounts of SOA formation were observed. We recommend the OFR185 mode for future forest studies. Concurrent gas-phase measurements of air after OH oxidation illustrate the decay of primary VOCs, production of small oxidized organic compounds, and net production at lower ages followed by net consumption of terpenoid oxidation products as photochemical age increased. New particle formation was observed in the reactor after oxidation, especially during times when precursor gas concentrations and SOA formation were largest. Approximately 6 times more SOA was formed in the reactor from OH oxidation than could be explained by the VOCs measured in ambient air. Several recently-developed instruments quantified ambient semi- and intermediate-volatility organic compounds (S/IVOCs) that were not detected by a PTR-TOF-MS. An SOA yield of 24–80 % from those compounds can explain the observed SOA, suggesting that these typically unmeasured S/IVOCs play a substantial role in ambient SOA formation. Our results allow ruling out condensation sticking coefficients much lower than 1. Our measurements help clarify the magnitude of SOA formation in forested environments, and demonstrate methods for interpretation of ambient OFR measurements.

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