Grantee Research Project Results
Final Report: Highly Time-Resolved Source Apportionment Techniques for Organic Aerosols Using the Aerodyne Aerosol Mass Spectrometer
EPA Grant Number: R832161Title: Highly Time-Resolved Source Apportionment Techniques for Organic Aerosols Using the Aerodyne Aerosol Mass Spectrometer
Investigators: Jimenez, Jose-Luis , Schauer, James J. , Hannigan, Michael P. , Zhang, Qi
Institution: University of Colorado at Boulder , University of Wisconsin - Madison
EPA Project Officer: Chung, Serena
Project Period: December 1, 2004 through November 30, 2007 (Extended to November 30, 2008)
Project Amount: $450,000
RFA: Source Apportionment of Particulate Matter (2004) RFA Text | Recipients Lists
Research Category: Particulate Matter , Air Quality and Air Toxics , Air
Objective:
The overall objective of this research project was to develop, validate, and apply source apportionment techniques for organic aerosol (OA) measurements from the Aerodyne Aerosol Mass Spectrometer (AMS), as well as enhanced instrumental techniques that improve the characterization of OA with the AMS. The AMS is the only current real-time instrument that provides quantitative size-resolved organic aerosol data with a time resolution of a few minutes or better. Results prior to the start of the project indicated that AMS organic aerosol data were sufficiently specific to address the critical need for source apportionment of organic aerosols with very high time resolution. The primary results of this project were the demonstration and application of source apportionment techniques for organic aerosols with very high time resolution, and of several new techniques for OA analysis. The results of this project are having a rapid and broad impact, in part because the techniques developed here can be applied to datasets acquired by many researchers around the world, including the more than 50 research groups with an AMS. In addition, these techniques and algorithms will be useful for source apportionment using data from other emerging and future quantitative aerosol mass spectrometers.Summary/Accomplishments (Outputs/Outcomes):
This project had two major components: (1) the development and application of receptor model techniques to AMS OA data, and (2) the field deployment and field data analysis for several new techniques aimed at obtaining more chemically-specific OA information from the AMS for source apportionment purposes. Our work successfully met and exceeded the original goals of the project, as summarized below for each of the two major components.
(1) Progress in receptor model development and application
Several statistical source apportionment models for apportioning OA were investigated, including custom techniques that take advantage of our understanding of the data (Custom Principal Component Analysis, CPCA, and Multiple Component Analysis, MCA, both developed as part of this project), and a standard multivariate receptor model (Positive Matrix Factorization, PMF). Our work was the first to demonstrate that different organic components could be extracted from AMS field datasets, including their concentrations, mass spectra, diurnal cycles, and size distributions (and more recently elemental composition). The application of these techniques to AMS data has received very intense interest from the scientific community and in fact it has become an active subfield on its own. Results on these analyses have been presented at major national and international conferences, including an invited oral presentation at the Gordon Research Conference on Atmospheric Chemistry and a plenary lecture at the Annual Conference of the American Association on Aerosol Research (AAAR), both delivered by the PI. Sixteen publications on this topics and acknowledging this grant have been published or submitted (listed below), and many presentations have also been given at major meetings such as the AAAR, AGU, EAC, and EGU annual meetings. The papers presenting these results are having a significant impact, and they have already received more than 400 citations in ISI Web of Science (as of May 2009). Seven of the published papers have been classified as “Highly Cited Papers” (Top 1% citation in their journals) by ISI Web of Science, and two have been classified as “Top Cited Papers” by the journal Environmental Science and Technology. One is the most cited paper in Geophysical Research Letters since 2007 (of 3382 papers) and another is the most cited paper in Environmental Science and Technology since 2008 (of 2099 papers).
We first demonstrated all the techniques with the AMS data acquired at the EPA Pittsburgh Supersite in September 2002, resulting in several publications where we reported for the first time the direct identification of hydrocarbon-like organic aerosols (HOA) and oxygenated organic aerosols (OOA), which showed strong correspondence with primary and secondary organic aerosols (POA and SOA), respectively [Zhang et al., ES&T 2005; ACP 2005]. OOA was larger than HOA, contrary to previous results at this site. We also explored whether OOA increased during periods with high aerosol acidity, which could be a sign of acid-catalyzed SOA formation, and found that this increase was at most 25% and likely lower [Zhang et al., ES&T 2007]. We later published [Zhang et al., GRL, 2007] an MCA analysis of 37 highly timeresolved AMS datasets acquired in the Northern Hemisphere mid-latitudes in 11 urban areas, 5 regions downwind of urban areas, and 11 rural/remote locations (representative of high elevation, forested, pristine, and continentally-influenced marine atmospheres). At most sites the MCA retrieved several types of OOA. The results of this analysis strongly indicate that global models largely underestimated the importance of Secondary Organic Aerosols (SOA) and likely overestimated the importance of Primary Organic Aerosols (POA).
In addition to the work on custom source apportionment techniques just described, we also pursued the application of Positive Matrix Factorization (PMF), a source apportionment method commonly used in atmospheric science, to AMS datasets. We performed an in-depth evaluation of the proper specification of errors for AMS data, as well as the interpretation and pitfalls of PMF factorization of AMS data [Ulbrich et al., ACP 2009]. In particular we identified the tendency of PMF-AMS solutions to produce “split” factors which have realistic-looking time series and mass spectra, yet have no physical reality. We have developed the PMF Evaluation Panel (PET), an Igor-based software interface to automate the running and especially the analysis of PMF solutions. The code automatically generates the most useful plots to evaluate the results of the model and diagnostic statistics that help investigators investigate the range of solutions of the model. Systematic investigation of uncertainties is automated with bootstrapping, multiple seeds, and FPEAK variation [Ulbrich et al., ACP 2009]. The PET has been shared with the AMS and the wider research community starting at the AMS Users Meeting in Manchester, UK, in Sep. 2008, and about two dozen groups are using this software tool at present, greatly facilitating the application and consistent interpretation of this powerful but very complex technique.
The identification of spectra from statistical techniques necessitates the use of standard spectra for known sources. For this purpose, we created three public web-based mass spectral databases: the unit-resolution AMS database, the high-resolution AMS database, and the thermal-desorption / thermal denuder database (see e.g. http://cires.colorado.edu/jimenez-group/AMSsd/). These databases are growing as new spectra are added from our group and others in the AMS community, and now contain over 100 spectra or spectra/volatility profiles [Ulbrich et al., ACP 2009].
We have applied PMF and MCA to multiple datasets of our own and from collaborators. PMF was first applied to the Pittsburgh 2002 dataset, largely confirming the previously published CPCA results, but also identifying a small (8%) semivolatile OOA-2 component which correlates with nitrate and chloride while the main OOA-1 component correlates with particle sulfate instead and appears non-volatile [Ulbrich et al., ACP 2009]. Other publications on this area and acknowledging this grant include: (a) Takegawa et al. [JGR, 2006] obtains good agreement between the HOA & OOA estimated with the AMS for Tokyo and the CO-tracer method for SOA estimation; (b) Kondo et al. [2007] concludes that about 90% of the OOA in Tokyo is water soluble while HOA is water insoluble by comparison of AMS CPCA results with PILS-WSOC analysis; (c) Cottrell et al. [JGR, 2008] reports that OOA dominates the aerosol composition in rural New Hampshire, apparently due to SOA of both anthropogenic and biogenic origin; (d) Nemitz et al. [AS&T, 2008] use PMF with a mixed OA concentration / eddy covariance flux AMS dataset from Boulder, CO, to quantify the fluxes OOA-1, OOA-2, and HOA, and reports that while the more regional OOA-I is undergoing net deposition, the more local HOA and OOA-2 have a net emission flux at this location; (e) Johnson et al. [ES&T, 2008] compare the AMS OA with the OA estimated from Proton Elastic Scattering Analysis (PESA) measurements of hydrogen for the 2003 Mexico City Metropolitan Area (MCMA-2003), reporting that 75% of the OA evaporated before PESA analysis, and that the OOA correlates better with the remaining PESA OA, which is consistent with the lower volatility of this component deduced from thermal denuder measurements (below); (f) Fast et al. [ACP, 2009] evaluate the results from a 3-D model (WRF-CHEM) using our results from PMF of highresolution AMS data.
An important part of this project was to compare the results of AMS-PMF with other more established methods for OA source apportionment. We have reported good comparisons with results from chemical mass balance (CMB) of organic molecular markers for the MILAGRO and SOAR-1 datasets [Docherty et al., ES&T 2008; Aiken et al., ACPD 2009]. Good comparisons were also observed with the EC-tracer method [Zhang et al., ACP 2005; Docherty et al, ES&T 2008], the WSOC method [Kondo et al., JGR, 2007; Docherty et al., ES&T, 2008], and the COtracer method [Takegawa et al., JGR, 2006; Docherty et al., ES&T, 2008]. Further comparisons for the SOAR-1 dataset are in progress and will be presented in future publications.
(2) Deployment in Field Studies and Data Analysis of New Techniques
A major accomplishment of this project was the organization and performance of the SOAR-1 and SOAR-2 (Study of Organic Aerosol in Riverside, phases 1 & 2) field experiments. These studies were organized by Profs. Jimenez and Ziemann (UC-Riverside), with participation from Profs. Schauer, Hannigan, and Zhang, with a focus on characterizing organic aerosols with a variety of techniques. They were carried out at UC-Riverside, which is located in a polluted region downwind of Los Angeles that is heavily impacted by both primary and secondary aerosol. Although it was originally intended that this study would include only the UCR, CU, and Wisconsin groups, as word of our intentions spread, many other research groups became interested in making measurements with a variety of complementary methods during this period. As a result, during the SOAR-1 study (~July 15-Aug. 15, 2005) approximately 60 scientists from 17 universities and research institutes and companies participated in what is probably the most complete field study of organic aerosols using advanced techniques to date. During SOAR-2 (Nov. 1-24, 2005) about 20 scientists from 8 groups participated. More detailed information on the participants and measurements can be found at Study of Organic Aerosols in Riverside, Phase 2, Riverside, California Exit. Eighteen (18) papers have been published so far based on the data acquired in this campaign by all participating groups, and at least 6 more are submitted or in preparation.
AMS results indicate a very reproducible aerosol concentration and composition from day to day, with a similar diurnal cycle. Differences between weekday and weekends are observed, presumably due to changes in emissions. Five methods produce consistent results, indicating that OA during SOAR is overwhelmingly secondary in nature during a period of several weeks with moderate ozone concentrations, and that SOA is the single largest component of PM1 aerosol in Riverside. Average SOA contributions of >80% were observed during mid-day periods while minimum SOA contributions of ~50% were observed during peak morning traffic periods. A similar result holds for Pasadena during SOAR-1. These results are contrary to previous estimates of SOA throughout the Los Angeles Basin which reported that, other than during severe photochemical smog episodes, SOA was lower than primary OA. We have used the SOAR source apportionment results in a study of cloud condensation nuclei and cloud properties for urban aerosol [Cubison et al., ACP, 2008] showing that not just the composition but also the mixing state of OA is critical for successful CCN closure.
During SOAR-1, the Jimenez group deployed several new instrument combinations for organic aerosol analysis: (a) a new high-resolution time-of-flight aerosol mass spectrometer (HR-ToFAMS) was deployed in the field for the first time, to provide additional insight on the aerosol chemical composition by allowing the direct determination of the elemental composition of every peak in the spectrum of the AMS [DeCarlo et al., Anal. Chem. 2006]; (b) a thermal denuder (TD) system was used in front of an AMS and a scanning mobility particle sizer (SMPS) to characterize the coupled chemistry-volatility profiles [Huffman et al., AS&T 2008; ES&T 2009; ACPD 2009]; and (c) a variable-temperature AMS vaporizer was used some of the time in both the ToF-AMS and HR-ToF-AMS to provide additional insight on the thermal properties of the organic aerosol [Docherty et al., AAAR 2008]. These systems were used to continuously analyze ambient particles, and to analyze secondary organic aerosol (SOA) formed in several reactions carried out in the environmental chamber in the Ziemann laboratory.
The high-resolution analysis capability of the HR-ToF-AMS has enabled us to separate the inorganic from organic aerosol spectra, to enhance the spectral differences that are critical to the success of statistical methods such as PMF [Docherty et al., ES&T, 2008; Aiken et al., ACPD, 2009], and to develop a method for the direct measurement of organic elemental composition (O/C, N/C, H/C, and OM/OC) [Aiken et al., Anal. Chem. 2007; ES&T, 2008]. The latter paper applies the elemental analysis method for ambient, chamber, and laboratory biomass burning spectra, with results consistent with those of other techniques. One important result is that the OOA/SOA found in the atmosphere is significantly more oxygenated than the SOA made in traditional chamber experiments [Aiken et al., ES&T, 2008]. This difference decreases at lower precursor / SOA concentrations [Shilling et al., ACP, 2009], although at the expense of decreasing yields that increase the quantitative discrepancies with SOA concentrations in the field.
The thermal-denuder and variable vaporizer temperature data allow the separation of different OA components with different volatility behavior, as they enhance the contrast between them. Results from Mexico City and Riverside confirm that the least volatile OA component is OOA-1 (a surrogate for aged SOA) while HOA and OOA-2 (surrogate for fresh SOA) are more volatile. These results strongly support that all types of OA should be treated as semivolatile in models.
Two laboratory biomass burning experiments (FLAME-1 and FLAME-2 campaigns) that were carried out in 2006 and 2007 at the Missoula, MT Biomass Burning Chamber operated by the US Forest Service. The objective of this deployment was to obtain the first signatures of biomass burning aerosols using the HR-ToF-AMS and the thermal denuder. This experiment allowed us to obtain HR-ToF-AMS and thermal denuder signatures for smoke from 16 different biomasses at realistic dilution levels (1/10,000). During FLAME-2 we demonstrated a new high timeresolution (up to 100 Hz) mode of the ToF-AMS software that allows capturing rapid fluctuations on the emissions and easily separate flaming vs. smoldering emissions during stack burns. Results indicate a wide variability in the organic fraction, composition, and volatility across biomasses and burning conditions (flaming vs. smoldering). Biomass burning organic aerosols (BBOA) are oxygenated, but typically less than SOA. Most BBOA is also more more volatile than real-word SOA, and of similar volatility than urban POA [Aiken et al., ES&T 2008; Huffman et al., ES&T 2009]. The O/C of BBOA is on the range 0.3-0.45 [Huffman et al., ES&T, 2008], which are very similar to the values derived from PMF of ambient measurements [Aiken et al., ES&T, 2008].
An additional experiment was carried out with support from this project April/May 2007 to characterize the high-resolution and thermal denuder spectra from meat cooking, trash burning, and motor vehicle emissions. This experiment was motivated by questions arising from the analysis of the SOAR and MILAGRO campaigns. Mohr et al. [ES&T, 2009] and Huffman et al. [ES&T, 2009] present results of this experiment, which show with high resolution data that OA emitted by combustion engines and plastic burning are dominated by hydrocarbon-like (reduced) organic compounds. Meat cooking and especially paper burning contain significant fractions of oxygenated organic compounds; however, their unit-resolution mass spectral signatures are very similar to mass spectral signatures from hydrocarbon-like OA or primary OA, and very different from the mass spectra of ambient secondary or oxygenated OA (OOA). Thus, primary OA from any of these sources is very unlikely to be a significant direct source of ambient OOA. POA from all of these sources was semivolatile.
Another research topic was the development and application of a method allowing the first realtime determination of PAHs in submicron aerosols from aerosol mass spectrometry data [Marr et al., ACP, 2006; Dzepina et al., IJMS, 2007]. This technique was developed using data from the MCMA-2003 field study, and the AMS measurements showed good correlation with those from two separate techniques, but also identified some very reactive PAHs that are likely being destroyed by reaction artifacts on traditional filter-sampling techniques.
Finally a $15k supplement to this grant funded Prof. Weber of Georgia Tech for deploying two organic aerosol analysis techniques during SOAR-1, which have resulted in two publications [Peltier et al., AS&T 2007; Docherty et al., ES&T 2008].
Conclusions:
Several new techniques were developed and demonstrated in this project, which have been very rapidly adopted by many other groups in the research community, and which have been described in many highly-cited papers. We demonstrated for the first time factor analysis of AMS spectra to extract OA components, which has rapidly become an established technique, and which compared favorably to four other techniques at several locations. We have applied these techniques in many studies, and we have been able to show that SOA is often underestimated by traditional models. The high-resolution ToF-AMS and the OA elemental analysis based on its data allow acquiring this information with unprecedented sensitivity and time-resolution and with them we demonstrated that chamber SOA from traditional experiments is less oxygenated than ambient SOA. Thermal-denuder data showed that all OA types are semivolatile and that ambient POA is similarly or more volatile than ambient SOA. Finally emissions from biomass burning, meat cooking, and trash burning were characterized for the first time using an HR-ToFAMS.
Journal Articles on this Report : 31 Displayed | Download in RIS Format
Other project views: | All 115 publications | 31 publications in selected types | All 31 journal articles |
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Aiken AC, DeCarlo PF, Jimenez JL. Elemental analysis of organic species with electron ionization high-resolution mass spectrometry. Analytical Chemistry 2007;79(21):8350-8358. |
R832161 (2007) R832161 (Final) |
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Aiken AC, DeCarlo PF, Kroll JH, Worsnop DR, Huffman JA, Docherty KS, Ulbrich IM, Mohr C, Kimmel JR, Sueper D, Sun Y, Zhang Q, Trimborn A, Northway M, Ziemann PJ, Canagaratna MR, Onasch TB, Alfarra MR, Prevot ASH, Dommen J, Duplissy J, Metzger A, Baltensperger U, Jimenez JL. O/C and OM/OC ratios of primary, secondary, and ambient organic aerosols with high-resolution time-of-flight aerosol mass spectrometry. Environmental Science & Technology 2008;42(12):4478-4485. |
R832161 (Final) R831080 (Final) |
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Aiken AC, de Foy B, Wiedinmyer C, DeCarlo PF, Ulbrich IM, Wehrli MN, Szidat S, Prevot ASH, Noda J, Wacker L, Volkamer R, Fortner E, Wang J, Laskin A, Shutthanandan V, Zheng J, Zhang R, Paredes-Miranda G, Arnott WP, Molina LT, Sosa G, Querol X, Jimenez JL. Mexico City aerosol analysis during MILAGRO using high resolution aerosol mass spectrometry at the urban supersite (T0)-Part 1: Fine particle composition and organic source apportionment. Atmospheric Chemistry and Physics 2009;9(17):6633-6653. |
R832161 (Final) |
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Aiken AC, de Foy B, Wiedinmyer C, DeCarlo PF, Ulbrich IM, Wehrli MN, Szidat S, Prevot ASH, Noda J, Wacker L, Volkamer R, Fortner E, Wang J, Laskin A, Shutthanandan V, Zheng J, Zhang R, Paredes-Miranda G, Arnott WP, Molina LT, Sosa G, Querol X, Jimenez JL. Mexico City aerosol analysis during MILAGRO using high resolution aerosol mass spectrometry at the urban supersite (T0)-Part 2:Analysis of the biomass burning contribution and the non-fossil carbon fraction. Atmospheric Chemistry and Physics 2010;10(12):5315-5341. |
R832161 (Final) |
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Cottrell LD, Griffin RJ, Jimenez JL, Zhang Q, Ulbrich I, Ziemba LD, Beckman PJ, Sive BC, Talbot RW. Submicron particles at Thompson Farm during ICARTT measured using aerosol mass spectrometry. Journal of Geophysical Research-Atmospheres 2008;113(D8):D08212. |
R832161 (2007) R832161 (Final) |
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Cubison MJ, Ervens B, Feingold G, Docherty KS, Ulbrich IM, Shields L, Prather K, Hering S, Jimenez JL. The influence of chemical composition and mixing state of Los Angeles urban aerosol on CCN number and cloud properties. Atmospheric Chemistry and Physics 2008;8(18):5649-5667. |
R832161 (2007) R832161 (Final) R831080 (Final) |
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DeCarlo PF, Kimmel JR, Trimborn A, Northway MJ, Jayne JT, Aiken AC, Gonin M, Fuhrer K, Horvath T, Docherty KS, Worsnop DR, Jimenez JL. Field-deployable, high-resolution, time-of-flight aerosol mass spectrometer. Analytical Chemistry 2006;78(24):8281-8289. |
R832161 (2006) R832161 (2007) R832161 (Final) |
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DeCarlo PF, Ulbrich IM, Crounse J, de Foy B, Dunlea EJ, Aiken AC, Knapp D, Weinheimer AJ, Campos T, Wennberg PO, Jimenez JL. Investigation of the sources and processing of organic aerosol over the Central Mexican Plateau from aircraft measurements during MILAGRO. Atmospheric Chemistry and Physics 2010;10(12):5257-5280. |
R832161 (Final) R833747 (2010) R833747 (2011) R833747 (Final) |
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Docherty KS, Stone EA, Ulbrich IM, DeCarlo PF, Snyder DC, Schauer JJ, Peltier RE, Weber RJ, Murphy SM, Seinfeld JH, Grover BD, Eatough DJ, Jimenez JL. Apportionment of primary and secondary organic aerosols in southern California during the 2005 Study of Organic Aerosols in Riverside (SOAR-1). Environmental Science & Technology 2008;42(20):7655-7662. |
R832161 (Final) R831080 (Final) |
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Docherty KS, Aiken AC, Huffman JA, Ulbrich IM, DeCarlo PF, Sueper D, Worsnop DR, Snyder DC, Peltier RE, Weber RJ, Grover BD, Eatough DJ, Williams BJ, Goldstein AH, Ziemann PJ, Jimenez JL. The 2005 Study of Organic Aerosols at Riverside (SOAR-1): instrumental intercomparisons and fine particle composition. Atmospheric Chemistry and Physics 2011;11(23):12387-12420. |
R832161 (Final) R831080 (Final) |
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Dzepina K, Arey J, Marr LC, Worsnop DR, Salcedo D, Zhang Q, Onasch TB, Molina LT, Molina MJ, Jimenez JL. Detection of particle-phase polycyclic aromatic hydrocarbons in Mexico City using an aerosol mass spectrometer. International Journal of Mass Spectrometry 2007;263(2-3):152-170. |
R832161 (2006) R832161 (2007) R832161 (Final) |
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Dzepina K, Volkamer RM, Madronich S, Tulet P, Ulbrich IM, Zhang Q, Cappa CD, Ziemann PJ, Jimenez JL. Evaluation of recently-proposed secondary organic aerosol models for a case study in Mexico City. Atmospheric Chemistry and Physics 2009;9(15):5681-5709. |
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Fast J, Aiken AC, Allan J, Alexander L, Campos T, Canagaratna MR, Chapman E, DeCarlo PF, de Foy B, Gaffney J, de Gouw J, Doran JC, Emmons L, Hodzic A, Herndon SC, Huey G, Jayne JT, Jimenez JL, Kleinman L, Kuster W, Marley N, Russell L, Ochoa C, Onasch TB, Pekour M, Song C, Ulbrich IM, Warneke C, Welsh-Bon D, Wiedinmyer C, Worsnop DR, Yu X-Y, Zaveri R. Evaluating simulated primary anthropogenic and biomass burning organic aerosols during MILAGRO:implications for assessing treatments of secondary organic aerosols. Atmospheric Chemistry and Physics 2009;9(16):6191-6215. |
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Huffman JA, Ziemann PJ, Jayne JT, Worsnop DR, Jimenez JL. Development and characterization of a fast-stepping/scanning thermodenuder for chemically-resolved aerosol volatility measurements. Aerosol Science & Technology 2008;42(5):395-407. |
R832161 (2007) R832161 (Final) R831080 (Final) R833747 (Final) |
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Huffman JA, Docherty KS, Mohr C, Cubison MJ, Ulbrich IM, Ziemann PJ, Onasch TB, Jimenez JL. Chemically-resolved volatility measurements of organic aerosol from different sources. Environmental Science & Technology 2009;43(14):5351-5357. |
R832161 (Final) R831080 (Final) R833747 (2008) R833747 (2009) R833747 (Final) |
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Huffman JA, Docherty KS, Aiken AC, Cubison MJ, Ulbrich IM, DeCarlo PF, Sueper D, Jayne JT, Worsnop DR, Ziemann PJ, Jimenez JL. Chemically-resolved aerosol volatility measurements from two megacity field studies. Atmospheric Chemistry and Physics 2009;9(18):7161-7182. |
R832161 (Final) R831080 (Final) R833747 (2008) R833747 (Final) |
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Jimenez JL, Canagaratna MR, Donahue NM, Prevot AS, Zhang Q, Kroll JH, DeCarlo PF, Allan JD, Coe H, Ng NL, Aiken AC, Docherty KS, Ulbrich IM, Grieshop AP, Robinson AL, Duplissy J, Smith JD, Wilson KR, Lanz VA, Hueglin C, Sun YL, Tian J, Laaksonen A, Raatikainen T, Rautiainen J, Vaattovaara P, Ehn M, Kulmala M, Tomlinson JM, Collins DR, Cubison MJ, Dunlea EJ, Huffman JA, Onasch TB, Alfarra MR, Williams PI, Bower K, Kondo Y, Schneider J, Drewnick F, Borrmann S, Weimer S, Demerjian K, Salcedo D, Cottrell L, Griffin R, Takami A, Miyoshi T, Hatakeyama S, Shimono A, Sun JY, Zhang YM, Dzepina K, Kimmel JR, Sueper D, Jayne JT, Herndon SC, Trimborn AM, Williams LR, Wood EC, Middlebrook AM, Kolb CE, Baltensperger U, Worsnop DR. Evolution of organic aerosols in the atmosphere. Science 2009;326(5959):1525-1529. |
R832161 (Final) R831080 (Final) R833746 (2009) R833746 (2010) R833746 (Final) R833747 (Final) R833748 (2010) R833748 (Final) |
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Johnson KS, Laskin A, Jimenez JL, Shutthanandan V, Molina LT, Salcedo D, Dzepina K, Molina MJ. Comparative analysis of urban atmospheric aerosol by particle-induced X-ray emission (PIXE), proton elastic scattering analysis (PESA), and aerosol mass spectrometry (AMS). Environmental Science & Technology 2008;42(17):6619-6624. |
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Kondo Y, Miyazaki Y, Takegawa N, Miyakawa T, Weber RJ, Jimenez JL, Zhang Q, Worsnop DR. Oxygenated and water-soluble organic aerosols in Tokyo. Journal of Geophysical Research-Atmospheres 2007;112(D1):D01203. |
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Mohr C, Huffman JA, Cubison MJ, Aiken AC, Docherty KS, Kimmel JR, Ulbrich IM, Hannigan M, Jimenez JL. Characterization of primary organic aerosol emissions from meat cooking, trash burning, and motor vehicles with high-resolution aerosol mass spectrometry and comparison with ambient and chamber observations. Environmental Science & Technology 2009;43(7):2443-2449. |
R832161 (Final) R831080 (Final) |
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Nemitz E, Jimenez JL, Huffman JA, Ulbrich IM, Canagaratna MR, Worsnop DR, Guenther AB. An eddy-covariance system for the measurement of surface/atmosphere exchange fluxes of submicron aerosol chemical species—first application above an urban area. Aerosol Science & Technology 2008;42(8):636-657. |
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Sheesley RJ, Deminter JT, Meiritz M, Snyder DC, Schauer JJ. Temporal trends in motor vehicle and secondary organic tracers using in situ methylation thermal desorption GCMS. Environmental Science & Technology 2010;44(24):9398-9404. |
R832161 (Final) R831080 (Final) R831088 (Final) |
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Shilling JE, Chen Q, King SM, Rosenoern T, Kroll JH, Worsnop DR, DeCarlo PF, Aiken AC, Sueper D, Jimenez JL, Martin ST. Loading-dependent elemental composition of α-pinene SOA particles. Atmospheric Chemistry and Physics 2009;9(3):771-782. |
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Snyder DC, Schauer JJ. An Inter-comparison of two black carbon aerosol instruments and a semi-continuous elemental carbon instrument in the urban environment. Aerosol Science and Technology 2007;41(5):463-474. |
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Takegawa N, Miyakawa T, Kondo Y, Jimenez JL, Zhang Q, Worsnop DR, Fukuda M. Seasonal and diurnal variations of submicron organic aerosol in Tokyo observed using the Aerodyne aerosol mass spectrometer (AMS). Journal of Geophysical Research-Atmospheres 2006;111(D11):D11206. |
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Ulbrich IM, Canagaratna MR, Zhang Q, Worsnop DR, Jimenez JL. Interpretation of organic components from Positive Matrix Factorization of aerosol mass spectrometric data. Atmospheric Chemistry and Physics 2009;9(9):2891-2918. |
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Williams BJ, Goldstein AH, Kreisberg NM, Hering SV, Worsnop DR, Ulbrich IM, Docherty KS, Jimenez JL. Major components of atmospheric organic aerosol in southern California as determined by hourly measurements of source marker compounds. Atmospheric Chemistry and Physics 2010;10(23):11577-11603. |
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Zhang Q, Worsnop DR, Canagaratna MR, Jimenez JL. Hydrocarbon-like and oxygenated organic aerosols in Pittsburgh: insights into sources and processes of organic aerosols. Atmospheric Chemistry and Physics 2005;5(12):3289-3311. |
R832161 (2005) R832161 (2006) R832161 (2007) R832161 (Final) R831080 (Final) |
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Zhang Q, Alfarra MR, Worsnop DR, Allan JD, Coe H, Canagaratna MR, Jimenez JL. Deconvolution and quantification of hydrocarbon-like and oxygenated organic aerosols based on aerosol mass spectrometry. Environmental Science & Technology 2005;39(13):4938-4952. |
R832161 (2005) R832161 (2006) R832161 (2007) R832161 (Final) R831080 (Final) |
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Zhang Q, Jimenez JL, Canagaratna MR, Allan JD, Coe H, Ulbrich I, Alfarra MR, Takami A, Middlebrook AM, Sun YL, Dzepina K, Dunlea E, Docherty K, DeCarlo PF, Salcedo D, Onasch T, Jayne JT, Miyoshi T, Shimono A, Hatakeyama S, Takegawa N, Kondo Y, Schneider J, Drewnick F, Borrmann S, Weimer S, Demerjian K, Williams P, Bower K, Bahreini R, Cottrell L, Griffin RJ, Rautiainen J, Sun JY, Zhang YM, Worsnop DR. Ubiquity and dominance of oxygenated species in organic aerosols in anthropogenically-influenced Northern Hemisphere midlatitudes. Geophysical Research Letters 2007;34(13):L13801. |
R832161 (2007) R832161 (Final) R831080 (Final) R831454 (Final) |
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Zhang Q, Jimenez JL, Worsnop DR, Canagaratna M. A case study of urban particle acidity and its influence on secondary organic aerosol. Environmental Science & Technology 2007;41(9):3213-3219. |
R832161 (2006) R832161 (2007) R832161 (Final) |
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Supplemental Keywords:
ambient air, tropospheric air pollution, particulates, environmental chemistry, monitoring, carbonaceous particles, combustion aerosols, source apportionment, primary organic aerosols, secondary organic aerosols, ToF-AMS, thermal denuder;, RFA, Scientific Discipline, Air, Ecosystem Protection/Environmental Exposure & Risk, particulate matter, Air Quality, Environmental Chemistry, Monitoring/Modeling, Environmental Monitoring, Environmental Engineering, particulate organic carbon, atmospheric dispersion models, atmospheric measurements, model-based analysis, time resolved apportionment, source apportionment, chemical characteristics, emissions monitoring, environmental measurement, airborne particulate matter, air quality models, air quality model, air sampling, speciation, particulate matter mass, analytical chemistry, aerodyne aerosol mass spectrometry, monitoring of organic particulate matter, modeling studies, chemical transport models, real-time monitoring, aerosol analyzers, chemical speciation sampling, particle size measurementRelevant Websites:
Prof. Jose-Luis Jimenez & Group Web Page ExitStudy of Organic Aerosols in Riverside, Phase 2, Riverside, California Exit
AMS Spectral Database (Unit Mass Resolution) Exit
Combined Mass Spectra & Volatility Database Exit
High Resolution AMS Spectral Database Exit
Igor Data Analysis for HDF Files (SQUIRREL) Exit
ToF-AMS Analysis Software Exit
James Jay Schauer, Professor Exit
Mike Hannigan, Assistant Professor Exit
Qi Zhang, Associate Professor Exit
Progress and Final Reports:
Original AbstractThe perspectives, information and conclusions conveyed in research project abstracts, progress reports, final reports, journal abstracts and journal publications convey the viewpoints of the principal investigator and may not represent the views and policies of ORD and EPA. Conclusions drawn by the principal investigators have not been reviewed by the Agency.