Articles | Volume 6, issue 4
Development and technical paper 18 Jul 2013
Development and technical paper | 18 Jul 2013
Improving the representation of secondary organic aerosol (SOA) in the MOZART-4 global chemical transport model
A. Mahmud and K. Barsanti
No articles found.
Qi Li, Jia Jiang, Isaac Afreh, Kelley C. Barsanti, and David R. Cocker III
Atmos. Chem. Phys. Discuss.,
Preprint under review for ACPShort summary
The chamber-derived SOA yields from camphene are reported for the first time. The role of peroxy radicals (RO2) was investigated using chemically detailed box models. We observed higher SOA yields (up to 64 %) in the experiments with added NOx than without, due to the formation of highly oxygenated organic molecules (HOMs) when NOx is present. This work can improve the representation of camphene in air quality models and provide insights into other monoterpene studies.
Zachary C. J. Decker, Michael A. Robinson, Kelley C. Barsanti, Ilann Bourgeois, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Frank M. Flocke, Alessandro Franchin, Carley D. Fredrickson, Samuel R. Hall, Hannah Halliday, Christopher D. Holmes, L. Gregory Huey, Young Ro Lee, Jakob Lindaas, Ann M. Middlebrook, Denise D. Montzka, Richard H. Moore, J. Andrew Neuman, John B. Nowak, Brett B. Palm, Jeff Peischl, Pamela S. Rickly, Andrew W. Rollins, Thomas B. Ryerson, Rebecca H. Schwantes, Lee Thornhill, Joel A. Thornton, Geoff S. Tyndall, Kirk Ullmann, Paul Van Rooy, Patrick R. Veres, Andrew J. Weinheimer, Elizabeth Wiggins, Edward Winstead, Caroline Womack, and Steven S. Brown
Atmos. Chem. Phys. Discuss.,
Preprint under review for ACPShort summary
To understand air quality impacts from wildfire smoke we need an accurate picture of how wildfire smoke changes chemically both day and night as sunlight changes the chemistry of smoke. We present a chemical analysis of wildfire smoke as it changes from midday through the night. We use aircraft observations from the FIREX-AQ field campaign with a chemical box model. We find that even under sunlight typical “nighttime” chemistry thrives and controls the fate of key smoke plume chemical processes.
Sabrina Chee, Kelley Barsanti, James N. Smith, and Nanna Myllys
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
We explored molecular properties affecting atmospheric particle formation efficiency and derived a parameterization between particle formation rate and heterodimer concentration, which showed good agreement to previously reported experimental data. Considering the simplicity of calculating heterodimer concentration, this approach has potential to improve estimates of global cloud condensation nuclei in models that are limited by the computational expense of calculating particle formation rate.
Isaac Kwadjo Afreh, Bernard Aumont, Marie Camredon, and Kelley Claire Barsanti
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
This is the first SOA modeling study of the ubiquitous but understudied monoterpene, camphene. The explicit chemical model GECKO-A represented chamber data for two well-studied monoterpenes. The predicted camphene SOA yield was relatively high in comparison, ~2× α-pinene. Using 50 / 50 α-pinene / limonene as a surrogate for camphene increased predicted SOA mass from biomass burning fuels by up to ~100 %. The accurate representation of camphene in air quality models can improve predictions of SOA.
Dagny A. Ullmann, Mallory L. Hinks, Adrian M. Maclean, Christopher L. Butenhoff, James W. Grayson, Kelley Barsanti, Jose L. Jimenez, Sergey A. Nizkorodov, Saeid Kamal, and Allan K. Bertram
Atmos. Chem. Phys., 19, 1491–1503,Short summary
We measured the viscosity and diffusion of organic molecules in secondary organic aerosol (SOA) generated from the ozonolysis of limonene. The results suggest that the mixing times of large organics in the SOA studied are short (< 1 h) for conditions found in the planetary boundary layer. The results also show that the Stokes–Einstein equation gives accurate predictions of diffusion coefficients of large organics within the studied SOA up to a viscosity of 102 to 104 Pa s.
Coty N. Jen, Lindsay E. Hatch, Vanessa Selimovic, Robert J. Yokelson, Robert Weber, Arantza E. Fernandez, Nathan M. Kreisberg, Kelley C. Barsanti, and Allen H. Goldstein
Atmos. Chem. Phys., 19, 1013–1026,Short summary
Wildfires in the western US are occurring more frequently and burning larger land areas. Smoke from these fires will play a greater role in regional air quality and atmospheric chemistry than in the past. To help fire and climate modelers and atmospheric experimentalists better understand how smoke impacts the environment, we have separated, identified, classified, and quantified the thousands of organic compounds found in smoke and related their amounts emitted to fire conditions.
Lindsay E. Hatch, Albert Rivas-Ubach, Coty N. Jen, Mary Lipton, Allen H. Goldstein, and Kelley C. Barsanti
Atmos. Chem. Phys., 18, 17801–17817,Short summary
We demonstrate the use of solid-phase extraction (SPE) disks for the untargeted analysis of gas-phase intermediate volatility and semi-volatile organic compounds emitted from biomass burning. SPE and Teflon filter samples collected from laboratory fires were analyzed by two-dimensional gas chromatography, with distinct differences in the observed chromatographic profiles as a function of fuel type. Fuel-dependent emissions and volatility differences among benzenediol isomers were captured.
Adrian M. Maclean, Christopher L. Butenhoff, James W. Grayson, Kelley Barsanti, Jose L. Jimenez, and Allan K. Bertram
Atmos. Chem. Phys., 17, 13037–13048,Short summary
Using laboratory data, meteorological fields and a chemical transport model, we investigated how often mixing times are < 1 h within SOA in the planetary boundary layer (PBL). Based on viscosity data for alpha-pinene SOA generated using mass concentrations of ~1000 µg m −3, mixing times in biogenic SOA are < 1h most of the time.
Qijing Bian, Shantanu H. Jathar, John K. Kodros, Kelley C. Barsanti, Lindsay E. Hatch, Andrew A. May, Sonia M. Kreidenweis, and Jeffrey R. Pierce
Atmos. Chem. Phys., 17, 5459–5475,Short summary
In this paper, we perform simulations of the evolution of biomass-burning organic aerosol in laboratory smog-chamber experiments and ambient plumes. We find that in smog-chamber experiments, vapor wall losses lead to a large reduction in the apparent secondary organic aerosol formation. In ambient plumes, fire size and meteorology regulate the plume dilution rate, primary organic aerosol evaporation rate, and secondary organic aerosol formation rate.
Lindsay E. Hatch, Robert J. Yokelson, Chelsea E. Stockwell, Patrick R. Veres, Isobel J. Simpson, Donald R. Blake, John J. Orlando, and Kelley C. Barsanti
Atmos. Chem. Phys., 17, 1471–1489,Short summary
The most comprehensive database of gaseous biomass burning emissions to date was compiled. Four complementary instruments were deployed together during laboratory fires. The results generally compared within experimental uncertainty and highlighted that a range of measurement approaches are required for adequate characterization of smoke composition. Observed compounds were binned based on volatility, and priority recommendations were made to improve secondary organic aerosol predictions.
Anna L. Hodshire, Michael J. Lawler, Jun Zhao, John Ortega, Coty Jen, Taina Yli-Juuti, Jared F. Brewer, Jack K. Kodros, Kelley C. Barsanti, Dave R. Hanson, Peter H. McMurry, James N. Smith, and Jeffery R. Pierce
Atmos. Chem. Phys., 16, 9321–9348,Short summary
Processes that control the growth of newly formed particles are not well understood and limit predictions of aerosol climate impacts. We combine state-of-the-art measurements at a central-US site with a particle-growth model to investigate the species and processes contributing to growth. Observed growth was dominated by organics, sulfate salts, or a mixture of these two. The model qualitatively captures the variability between different days.
T. Yli-Juuti, K. Barsanti, L. Hildebrandt Ruiz, A.-J. Kieloaho, U. Makkonen, T. Petäjä, T. Ruuskanen, M. Kulmala, and I. Riipinen
Atmos. Chem. Phys., 13, 12507–12524,
K. C. Barsanti, A. G. Carlton, and S. H. Chung
Atmos. Chem. Phys., 13, 12073–12088,
M. Xie, K. C. Barsanti, M. P. Hannigan, S. J. Dutton, and S. Vedal
Atmos. Chem. Phys., 13, 7381–7393,
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Geosci. Model Dev., 14, 3317–3333,Short summary
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Sara M. Blichner, Moa K. Sporre, Risto Makkonen, and Terje K. Berntsen
Geosci. Model Dev., 14, 3335–3359,Short summary
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Timothy Glotfelty, Diana Ramírez-Mejía, Jared Bowden, Adrian Ghilardi, and J. Jason West
Geosci. Model Dev., 14, 3215–3249,Short summary
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Mario Eduardo Gavidia-Calderón, Sergio Ibarra-Espinosa, Youngseob Kim, Yang Zhang, and Maria de Fatima Andrade
Geosci. Model Dev., 14, 3251–3268,Short summary
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Xiaoli G. Larsén and Jana Fischereit
Geosci. Model Dev., 14, 3141–3158,Short summary
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Pavel Krč, Jaroslav Resler, Matthias Sühring, Sebastian Schubert, Mohamed H. Salim, and Vladimír Fuka
Geosci. Model Dev., 14, 3095–3120,Short summary
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Tao Zheng, Sha Feng, Kenneth J. Davis, Sandip Pal, and Josep-Anton Morguí
Geosci. Model Dev., 14, 3037–3066,Short summary
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Audrey Fortems-Cheiney, Isabelle Pison, Grégoire Broquet, Gaëlle Dufour, Antoine Berchet, Elise Potier, Adriana Coman, Guillaume Siour, and Lorenzo Costantino
Geosci. Model Dev., 14, 2939–2957,Short summary
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James Hocking, Jérôme Vidot, Pascal Brunel, Pascale Roquet, Bruna Silveira, Emma Turner, and Cristina Lupu
Geosci. Model Dev., 14, 2899–2915,Short summary
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K. Wyat Appel, Jesse O. Bash, Kathleen M. Fahey, Kristen M. Foley, Robert C. Gilliam, Christian Hogrefe, William T. Hutzell, Daiwen Kang, Rohit Mathur, Benjamin N. Murphy, Sergey L. Napelenok, Christopher G. Nolte, Jonathan E. Pleim, George A. Pouliot, Havala O. T. Pye, Limei Ran, Shawn J. Roselle, Golam Sarwar, Donna B. Schwede, Fahim I. Sidi, Tanya L. Spero, and David C. Wong
Geosci. Model Dev., 14, 2867–2897,Short summary
This paper details the scientific updates in the recently released CMAQ version 5.3 (and v5.3.1) and also includes operational and diagnostic evaluations of CMAQv5.3.1 against observations and the previous version of the CMAQ (v5.2.1). This work was done to improve the underlying science in CMAQ. This article is used to inform the CMAQ modeling community of the updates to the modeling system and the expected change in model performance from these updates (versus the previous model version).
Ziyu Huang, Lei Zhong, Yaoming Ma, and Yunfei Fu
Geosci. Model Dev., 14, 2827–2841,Short summary
Spectral nudging is an effective dynamical downscaling method used to improve precipitation simulations of regional climate models (RCMs). However, the biases of the driving fields over the Tibetan Plateau (TP) would possibly introduce extra biases when spectral nudging is applied. The results show that the precipitation simulations were significantly improved when limiting the application of spectral nudging toward the potential temperature and water vapor mixing ratio over the TP.
Eve-Agnès Fiorentino, Henri Wortham, and Karine Sartelet
Geosci. Model Dev., 14, 2747–2780,Short summary
Indoor air quality (IAQ) is strongly influenced by reactivity with surfaces, which is called heterogeneous reactivity. To date, this reactivity is barely integrated into numerical models due to the strong uncertainties it is subjected to. In this work, an open-source IAQ model, called the H2I model, is developed to consider both gas-phase and heterogeneous reactivity and simulate indoor concentrations of inorganic compounds.
Yann Cohen, Virginie Marécal, Béatrice Josse, and Valérie Thouret
Geosci. Model Dev., 14, 2659–2689,Short summary
Assessing long-term chemistry–climate simulations with in situ and frequent observations near the tropopause is possible with the IAGOS commercial aircraft data set. This study presents a method that distributes the IAGOS data (ozone and CO) on a monthly model grid, limiting the impact of resolution for the evaluation of the modelled chemical fields. We applied it to the CCMI REF-C1SD simulation from the MOCAGE CTM and notably highlighted well-reproduced O3 behaviour in the lower stratosphere.
Vikram Khade, Saroja M. Polavarapu, Michael Neish, Pieter L. Houtekamer, Dylan B. A. Jones, Seung-Jong Baek, Tai-Long He, and Sylvie Gravel
Geosci. Model Dev., 14, 2525–2544,Short summary
A new modeling system has been developed at Environment and Climate Change Canada to ingest observations of carbon monoxide (CO) into a coupled weather and constituent transport model. We show that accounting for the uncertainty in surface flux leads to a better estimate of CO distributions. The benefit of assimilating observations from different simulated networks varies with region. This is the first step towards developing a state and flux estimation system for greenhouse gases.
Dongqi Lin, Basit Khan, Marwan Katurji, Leroy Bird, Ricardo Faria, and Laura E. Revell
Geosci. Model Dev., 14, 2503–2524,Short summary
We present an open-source toolbox WRF4PALM, which enables weather dynamics simulation within urban landscapes. WRF4PALM passes meteorological information from the popular Weather Research and Forecasting (WRF) model to the turbulence-resolving PALM model system 6.0. WRF4PALM can potentially extend the use of WRF and PALM with realistic boundary conditions to any part of the world. WRF4PALM will help study air pollution dispersion, wind energy prospecting, and high-impact wind forecasting.
Daniel M. Gilford
Geosci. Model Dev., 14, 2351–2369,Short summary
Potential intensity (PI) is a tropical cyclone's maximum speed limit given by modeling the storm as a thermal heat engine. pyPI is the first software package fully documenting the PI algorithm and translating it to Python. This study details/validates the underlying PI model and demonstrates its use in tropical cyclone intensity research. pyPI supports open science and transparency in the tropical meteorological community and is ideally suited for ongoing community development and improvement.
Mizuo Kajino, Makoto Deushi, Tsuyoshi Thomas Sekiyama, Naga Oshima, Keiya Yumimoto, Taichu Yasumichi Tanaka, Joseph Ching, Akihiro Hashimoto, Tetsuya Yamamoto, Masaaki Ikegami, Akane Kamada, Makoto Miyashita, Yayoi Inomata, Shin-ichiro Shima, Pradeep Khatri, Atsushi Shimizu, Hitoshi Irie, Kouji Adachi, Yuji Zaizen, Yasuhito Igarashi, Hiromasa Ueda, Takashi Maki, and Masao Mikami
Geosci. Model Dev., 14, 2235–2264,Short summary
This study compares performance of aerosol representation methods of the Japan Meteorological Agency's regional-scale nonhydrostatic meteorology–chemistry model (NHM-Chem). It indicates separate treatment of sea salt and dust in coarse mode and that of light-absorptive and non-absorptive particles in fine mode could provide accurate assessments on aerosol feedback processes.
Langwen Huang and David Topping
Geosci. Model Dev., 14, 2187–2203,Short summary
As our knowledge and understanding of atmospheric aerosol particle evolution and impact grows, designing community mechanistic models requires an ability to capture increasing chemical, physical and therefore numerical complexity. As the landscape of computing software and hardware evolves, it is important to profile the usefulness of emerging platforms in tackling this complexity. With this in mind we present JlBox v1.1, written in Julia.
Matthias Faust, Ralf Wolke, Steffen Münch, Roger Funk, and Kerstin Schepanski
Geosci. Model Dev., 14, 2205–2220,Short summary
Trajectory dispersion models are powerful and intuitive tools for tracing air pollution through the atmosphere. But the turbulent nature of the atmospheric boundary layer makes it challenging to provide accurate predictions near the surface. To overcome this, we propose an approach using wind and turbulence information at high temporal resolution. Finally, we demonstrate the strength of our approach in a case study on dust emissions from agriculture.
Jie Luo, Yongming Zhang, and Qixing Zhang
Geosci. Model Dev., 14, 2113–2126,Short summary
In this work, we developed a numerical method to investigate the effects of black carbon (BC) morphology on the estimation of brown carbon (BrC) absorption using the absorption Ångström exponent (AAE) method. We found that BC morphologies have significant impacts on the estimated BrC absorptions. Moreover, we have demonstrated under what conditions the AAE methods can provide good or bad estimations and explored the reasons for why the good or bad estimations were caused.
Georgia N. Theodoritsi, Giancarlo Ciarelli, and Spyros N. Pandis
Geosci. Model Dev., 14, 2041–2055,Short summary
Two schemes based on the volatility basis set were used for the simulation of biomass burning organic aerosol (bbOA) in the continental US. The first is the default scheme of the PMCAMx-SR model, and the second is a recently developed scheme based on laboratory experiments. The alternative bbOA scheme predicts much higher concentrations. The default scheme performed better during summer and fall, while the alternative scheme was a little better during spring.
James Weber, Scott Archer-Nicholls, Nathan Luke Abraham, Youngsub Matthew Shin, Thomas J. Bannan, Carl J. Percival, Asan Bacak, Paulo Artaxo, Michael Jenkin, M. Anwar H. Khan, Dudley E. Shallcross, Rebecca H. Schwantes, Jonathan Williams, and Alex T. Archibald
Geosci. Model Dev. Discuss.,
Revised manuscript accepted for GMDShort summary
The new mechanism CRI-Strat 2 features state-of-the-art isoprene chemistry, not previously available in UKCA, and improves UKCA’s ability to reproduce observed concentrations of isoprene, monoterpenes and OH in tropical regions. The enhanced ability to model isoprene, the most widely emitted non-methane volatile organic compound, will facilitate improved understanding into how isoprene and other BVOCs affect atmospheric composition and, through biosphere-atmosphere feedbacks, climate change.
Dana L. McGuffin, Yuanlong Huang, Richard C. Flagan, Tuukka Petäjä, B. Erik Ydstie, and Peter J. Adams
Geosci. Model Dev., 14, 1821–1839,Short summary
Atmospheric particle formation, emissions, and growth process rates are significant sources of uncertainty in predicting climate change. We aim to reduce that uncertainty by using measurements from several ground-based sites across Europe. We developed an estimation technique to adapt the governing process rates so model–measurement bias decays. The estimation framework developed has potential to improve model predictions while providing insight into the underlying atmospheric particle physics.
Harald Flentje, Ina Mattis, Zak Kipling, Samuel Rémy, and Werner Thomas
Geosci. Model Dev., 14, 1721–1751,Short summary
Atmospheric aerosols crucially impact air quality, climate and weather. Thus, global model forecasts of atmospheric constituents are published daily on the ECMWF website and are regularly verified by the CAMS service team. The IFS-AER model is largely able to reproduce observed 3-D distributions of the important particle types over Germany. The particle concentration is mostly captured within several tens of percent, but quantification of some specific processes still remains a challenge.
Lin Huang, Song Liu, Zeyuan Yang, Jia Xing, Jia Zhang, Jiang Bian, Siwei Li, Shovan Kumar Sahu, Shuxiao Wang, and Tie-Yan Liu
Geosci. Model Dev. Discuss.,
Revised manuscript accepted for GMDShort summary
Accurate estimation of emissions is the prerequisite for effectively controlling air pollution, while current methods either lack sufficient data or representation of nonlinearity. Here we proposed a novel deep learning method to model the dual relationship between emission and pollutant concentration. The emission can be updated through backpropagating the gradient of the loss function measuring the deviation between simulations and observations, resulting in a better model performance.
Edward C. Chan and Timothy M. Butler
Geosci. Model Dev. Discuss.,
Revised manuscript accepted for GMDShort summary
A large-eddy simulation based chemical transport model is implemented for an idealized street canyon. The dynamics of the model are evaluated using stationary measurements. A transient model run is also conducted over a 24-hour period, where variations of pollutant concentrations indicate dependence on emissions, background concentrations, and solar state. Comparison stationary model runs show changes in flow structures concentrations.
Jianhui Jiang, Imad El Haddad, Sebnem Aksoyoglu, Giulia Stefenelli, Amelie Bertrand, Nicolas Marchand, Francesco Canonaco, Jean-Eudes Petit, Olivier Favez, Stefania Gilardoni, Urs Baltensperger, and André S. H. Prévôt
Geosci. Model Dev., 14, 1681–1697,Short summary
We developed a box model with a volatility basis set to simulate organic aerosol (OA) from biomass burning and optimized the vapor-wall-loss-corrected OA yields with a genetic algorithm. The optimized parameterizations were then implemented in the air quality model CAMx v6.5. Comparisons with ambient measurements indicate that the vapor-wall-loss-corrected parameterization effectively improves the model performance in predicting OA, which reduced the mean fractional bias from −72.9 % to −1.6 %.
Oliver Branch, Thomas Schwitalla, Marouane Temimi, Ricardo Fonseca, Narendra Nelli, Michael Weston, Josipa Milovac, and Volker Wulfmeyer
Geosci. Model Dev., 14, 1615–1637,Short summary
Effective numerical weather forecasting is vital in arid regions like the United Arab Emirates where extreme events like heat waves, flash floods, and dust storms are becoming more severe. This study employs a high-resolution simulation with the WRF-NOAHMP model, and the output is compared with seasonal observation data from 50 weather stations. This type of verification is vital to identify model deficiencies and improve forecasting systems for arid regions.
Lukas Hubert Leufen, Felix Kleinert, and Martin G. Schultz
Geosci. Model Dev., 14, 1553–1574,Short summary
MLAir provides a coherent end-to-end structure for a typical time series analysis workflow using machine learning (ML). MLAir is adaptable to a wide range of ML use cases, focusing in particular on deep learning. The user has a free hand with the ML model itself and can select from different methods during preprocessing, training, and postprocessing. MLAir offers tools to track the experiment conduction, documents necessary ML parameters, and creates a variety of publication-ready plots.
Davide Ori, Leonie von Terzi, Markus Karrer, and Stefan Kneifel
Geosci. Model Dev., 14, 1511–1531,Short summary
Snowflakes have very complex shapes, and modeling their properties requires vast computing power. We produced a large number of realistic snowflakes and modeled their average properties by leveraging their fractal structure. Our approach allows modeling the properties of big ensembles of snowflakes, taking into account their natural variability, at a much lower cost. This enables the usage of remote sensing instruments, such as radars, to monitor the evolution of clouds and precipitation.
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