Development and initial evaluation of a dynamic species-resolved model for gas phase chemistry and size-resolved gas/particle partitioning associated with secondary organic aerosol formation

A module for predicting the dynamic evolution of the gas phase species and the aerosol size and composition distribution during formation of secondary organic aerosol (SOA) is presented. The module is based on the inorganic gas-aerosol equilibrium model Simulating the Composition of Atmospheric Particles at Equilibrium 2 (SCAPE2) and updated versions of the lumped Caltech Atmospheric Chemistry Mechanism (CACM) and the Model to Predict the Multiphase Partitioning of Organics (MPMPO). The aerosol phase generally consists of an organic phase and an aqueous phase containing dissolved inorganic and organic components. Simulations are presented in which a single salt (either dry or aqueous), a volatile organic compound, and oxides of nitrogen undergo photo-oxidation to form SOA. Predicted SOA mass yields for classes of aromatic and biogenic hydrocarbons exhibit the proper qualitative behavior when compared to laboratory chamber data. Inasmuch as it is currently not possible to represent explicitly aerosol phase chemistry involving condensed products of gas phase oxidation, the present model can be viewed as the most detailed SOA formation model available yet will undergo continued improvement in the future

Secondary organic aerosol 1. Atmospheric chemical mechanism for production of molecular constituents

This series of three papers addresses the representation of secondary organic aerosol (SOA) in atmospheric models. SOA forms when gas-phase organic species undergo oxidation, leading to products of sufficiently low vapor pressure that can partition between the gas and aerosol phases. The present paper, part 1, is devoted to the development of a gas-phase atmospheric chemical mechanism designed to represent ozone chemistry as well as formation of individual organic oxidation products that are capable of forming SOA. The ozone chemistry in the mechanism draws upon the recent work of Stockwell et al. [1997] and Jenkin et al. [1997] and SAPRC-97 and SAPRC-99 (available from W.P.L. Carter at http://helium.ucr.edu/~carter/). The mechanism is evaluated in the three-dimensional California Institute of Technology (CIT) model [Meng et al., 1998] by simulating gas-phase concentrations in the South Coast Air Basin (SoCAB) of California over the period 27–29 August 1987. Total predicted concentrations of gas-phase SOA compounds are compared with levels of SOA that have been inferred on the basis of ambient organic aerosol measurements during this period. These predicted concentrations indicate that the total gas-phase potential of SOA-forming compounds can account for observed aerosol concentrations. Part 2 develops a thermodynamic gas–aerosol partitioning module, and part 3 presents a full three-dimensional simulation of gas and aerosol levels in the SoCAB during a 1993 episode

Estimate of global atmospheric organic aerosol from oxidation of biogenic hydrocarbons

The results from a series of outdoor chamber experiments establishing the atmospheric aerosol-forming potential of fourteen terpenoid hydrocarbons have been used to estimate the annual amount of secondary organic aerosol formed globally from compounds emitted by vegetation. Hydroxyl radical, ozone, and nitrate radical oxidation each contribute to aerosol formation in full-photooxidation experiments; because oxidation by nitrate radical under ambient, remote conditions is likely to be negligible, parameters describing aerosol formation from hydroxyl radical and ozone reaction only are developed. Chamber results, temporally and spatially resolved, compound-specific estimates of biogenic hydrocarbon emissions, and hydroxyl radical and ozone fields are combined to lead to an estimate for atmospheric secondary organic aerosol formed annually from biogenic precursors of 18.5 Tg, a number smaller than the previously published estimate of 30–270 Tg [Andreae and Crutzen, 1997]

Gas-phase chemistry in the online multiscale NMMB/BSC Chemical Transport Model: Description and evaluation at global scale

This paper presents a comprehensive description and benchmark evaluation of the tropospheric gas-phase chemistry component of the NMMB/BSC Chemical Transport Model (NMMB/BSC-CTM), an online chemical weather prediction system conceived for both the regional and the global scale. We provide an extensive evaluation of a global annual cycle simulation using a variety of background surface stations (EMEP, WDCGG and CASTNET), ozonesondes (WOUDC, CMD and SHADOZ), aircraft data (MOZAIC and several campaigns), and satellite observations (SCIAMACHY and MOPITT). We also include an extensive discussion of our results in comparison to other state-of-the-art models. The model shows a realistic oxidative capacity across the globe. The seasonal cycle for CO is fairly well represented at different locations (correlations around 0.3–0.7 in surface concentrations), although concentrations are underestimated in spring and winter in the Northern Hemisphere, and are overestimated throughout the year at 800 and 500 hPa in the Southern Hemisphere. Nitrogen species are well represented in almost all locations, particularly NO2 in Europe (RMSE below 9 μg m−3). The modeled vertical distribution of NOx and HNO3 are in excellent agreement with the observed values and the spatial and seasonal trends of tropospheric NO2 columns correspond well to observations from SCIAMACHY, capturing the highly polluted areas and the biomass burning cycle throughout the year. Over Asia, the model underestimates NOx from March to August probably due to an underestimation of NOx emissions in the region. Overall, the comparison of the modelled CO and NO2 with MOPITT and SCIAMACHY observations emphasizes the need for more accurate emission rates from anthropogenic and biomass burning sources (i.e., specification of temporal variability). The resulting ozone (O3) burden (348 Tg) lies within the range of other state-of-the-art global atmospheric chemistry models. The model generally captures the spatial and seasonal trends of background surface O3 and its vertical distribution. However, the model tends to overestimate O3 throughout the troposphere in several stations. This is attributed to an overestimation of CO concentration over the southern hemisphere leading to an excessive production of O3. Overall, O3 correlations range between 0.6 to 0.8 for daily mean values. The overall performance of the NMMB/BSC-CTM is comparable to that of other state-of-the-art global chemical transport models.The authors wish to thank WOUDC, GAW, EMEP, WDCGG, CASTNET-EPA, NADP and EANET for the provision of measurement stations. Also, thanks go to the free use of the MOPITT CO data obtained from the NASA Langley Research Center Atmospheric Science Data Center. SCIAMACHY radiances have been provided by ESA. This work is funded by grants CGL2013-46736-R, Supercomputación and e-ciencia Project (CSD2007-0050) from the Consolider-Ingenio 2010 program of the Spanish Ministry of Economy and Competitiveness. Further support was provided by the SEV-2011-00067 grant of the Severo Ochoa Program, awarded by the Spanish Government. A.H. received funding from the Earth System Science Research School (ESSReS), an initiative of the Helmholtz Association of German research centres (HGF) at the AlfredWegener Institute for Polar and Marine Research. All the numerical simulations were performed with the MareNostrum Supercomputer hosted by the Barcelona Supercomputing Center. We also thank Beatriz Monge-Sanz for providing the COPCAT coefficients.Peer ReviewedPostprint (author's final draft

Secondary organic aerosol 3. Urban/regional scale model of size- and composition-resolved aerosols

The California Institute of Technology (CIT) three-dimensional urban/regional atmospheric model is used to perform comprehensive gas- and aerosol-phase simulations of the 8 September 1993 smog episode in the South Coast Air Basin of California (SoCAB) using the atmospheric chemical mechanism of part 1 [Griffin et al., 2002] and the thermodynamic module of part 2 [Pun et al., 2002]. This paper focuses primarily on simulations of secondary organic aerosol (SOA) and determination of the species and processes that lead to this SOA. Meteorological data and a gas and particulate emissions inventory for this episode were supplied directly by the South Coast Air Quality Management District. A summer 1993 atmospheric sampling campaign provides data against which the performance of the model is evaluated. Predictions indicate that SOA formation in the SoCAB is dominated by partitioning of hydrophobic secondary products of the oxidation of anthropogenic organics. The biogenic contribution to total SOA increases in the more rural eastern portions of the region, as does the fraction of hydrophilic SOA, the latter reflecting the increasing degree of oxidation of SOA species with atmospheric residence time

A methodology for developing Distributed Generation scenarios in urban areas using geographical information systems

The implementation of Distributed Generation (DG) may lead to increased pollutant emissions that adversely affect air quality. This work presents a systematic methodology to characterise DG installation in urban basins. First, a set of parameters that characterise a DG implementation scenario is described. Second, a general approach using Geographic Information Systems (GIS) data is presented. Third, the methodology is demonstrated by application to the South Coast Air Basin (SoCAB) of California. Results show that realistic scenarios in the SoCAB concentrate DG technologies nearby industrial zones and introduce pollutant mass increments no larger than 0.43% with respect to baseline emissions.We graciously acknowledge the financial support of the California Energy Commission, sponsor of this work, and the significant leadership and contributions of Marla Mueller, our Contract Manager. M. Carreras and M. Medrano thank the continuing support of the Balsells-Generalitat de Catalunya Fellowship

Description and evaluation of the Multiscale Online Nonhydrostatic AtmospheRe CHemistry model (NMMB-MONARCH) version 1.0: gas-phase chemistry at global scale

This paper presents a comprehensive description and benchmark evaluation of the tropospheric gas-phase chemistry component of the Multiscale Online Nonhydrostatic AtmospheRe CHemistry model (NMMB-MONARCH), formerly known as NMMB/BSC-CTM, that can be run on both regional and global domains. Here, we provide an extensive evaluation of a global annual cycle simulation using a variety of background surface stations (EMEP, WDCGG and CASTNET), ozonesondes (WOUDC, CMD and SHADOZ), aircraft data (MOZAIC and several campaigns), and satellite observations (SCIAMACHY and MOPITT). We also include an extensive discussion of our results in comparison to other state-of-the-art models. We note that in this study, we omitted aerosol processes and some natural emissions (lightning and volcano emissions). The model shows a realistic oxidative capacity across the globe. The seasonal cycle for CO is fairly well represented at different locations (correlations around 0.3–0.7 in surface concentrations), although concentrations are underestimated in spring and winter in the Northern Hemisphere, and are overestimated throughout the year at 800 and 500 hPa in the Southern Hemisphere. Nitrogen species are well represented in almost all locations, particularly NO2 in Europe (root mean square error – RMSE – below 5 ppb). The modeled vertical distributions of NOx and HNO3 are in excellent agreement with the observed values and the spatial and seasonal trends of tropospheric NO2 columns correspond well to observations from SCIAMACHY, capturing the highly polluted areas and the biomass burning cycle throughout the year. Over Asia, the model underestimates NOx from March to August, probably due to an underestimation of NOx emissions in the region. Overall, the comparison of the modeled CO and NO2 with MOPITT and SCIAMACHY observations emphasizes the need for more accurate emission rates from anthropogenic and biomass burning sources (i.e., specification of temporal variability). The resulting ozone (O3) burden (348 Tg) lies within the range of other state-of-the-art global atmospheric chemistry models. The model generally captures the spatial and seasonal trends of background surface O3 and its vertical distribution. However, the model tends to overestimate O3 throughout the troposphere in several stations. This may be attributed to an overestimation of CO concentration over the Southern Hemisphere leading to an excessive production of O3 or to the lack of specific chemistry (e.g., halogen chemistry, aerosol chemistry). Overall, O3 correlations range between 0.6 and 0.8 for daily mean values. The overall performance of the NMMB-MONARCH is comparable to that of other state-of-the-art global chemistry models

The NMMB/BSC-CTM: a multiscale online chemical weather prediction system

Abstract: The model NMMB/BSC-CTM is a new fully on-line chemical weather prediction system under development at the Earth Sciences Department of the Barcelona Supercomputing Center in collaboration with several research institutions. The basis of the development is the NCEP new global/regional Nonhydrostatic Multiscale Model on the B grid (NMMB). Its unified nonhydrostatic dynamical core allows regional and global simulations and forecasts. A mineral dust module has been coupled within the NMMB. The new system, NMMB/BSCDUST, simulates the atmospheric life cycle of the eroded desert dust. The main characteristics are its on-line coupling of the dust scheme with the meteorological driver, the wide range of applications from meso to global scales, and the dust shortwave and longwave radiative feedbacks on meteorology. In order to complement such development, the BSC works also in the implementation of a fully on-line gas-phase chemical mechanism. Chemical species are advected and mixed at the corresponding time steps of the meteorological tracers using the same numerical scheme of the NMMB. Advection is Eulerian, positive definite and monotone. The final objective of the work is to develop a fully chemical weather prediction system, namely NMMB/BSC-CTM, able to resolve gas-aerosol-meteorology interactions from global to local scales. Future efforts will be oriented to incorporate a multi-component aerosol module within the system with the aim to solve the life-cycle of relevant aerosols at global scale (dust, sea salt, sulfate, black carbon and organic carbon). In the present contribution we describe the status of development of the system and first evaluation results of the gas-phase chemistry.Postprint (published version

Chemistry Across Multiple Phases (CAMP) version 1.0: an integrated multiphase chemistry model

A flexible treatment for gas- and aerosol-phase chemical processes has been developed for models of diverse scale, from box models up to global models. At the core of this novel framework is an “abstracted aerosol representation” that allows a given chemical mechanism to be solved in atmospheric models with different aerosol representations (e.g., sectional, modal, or particle-resolved). This is accomplished by treating aerosols as a collection of condensed phases that are implemented according to the aerosol representation of the host model. The framework also allows multiple chemical processes (e.g., gas- and aerosol-phase chemical reactions, emissions, deposition, photolysis, and mass transfer) to be solved simultaneously as a single system. The flexibility of the model is achieved by (1) using an object-oriented design that facilitates extensibility to new types of chemical processes and to new ways of representing aerosol systems, (2) runtime model configuration using JSON input files that permits making changes to any part of the chemical mechanism without recompiling the model (this widely used, human-readable format allows entire gas- and aerosol-phase chemical mechanisms to be described with as much complexity as necessary), and (3) automated comprehensive testing that ensures stability of the code as new functionality is introduced. Together, these design choices enable users to build a customized multiphase mechanism without having to handle preprocessors, solvers, or compilers. Removing these hurdles makes this type of modeling accessible to a much wider community, including modelers, experimentalists, and educators. This new treatment compiles as a stand-alone library and has been deployed in the particle-resolved PartMC model and in the Multiscale Online AtmospheRe CHemistry (MONARCH) chemical weather prediction system for use at regional and global scales. Results from the initial deployment to box models of different complexity and MONARCH will be discussed, along with future extension to more complex gas–aerosol systems and the integration of GPU-based solvers.Matthew L. Dawson has received funding from the European Union's Horizon 2020 research and innovation program under Marie Skłodowska-Curie grant agreement no. 747048. Matthew L. Dawson, Oriol Jorba, and Christian Guzman have been supported by the Ministerio de Ciencia, Innovación y Universidades (grant no. RTI2018-099894-BI00). Christian Guzman acknowledges funding from the AXA Research Fund. Nicole Riemer, Matthew West, and Jeffrey H. Curtis acknowledge funding from the National Science Foundation (grant no. AGS 19-41110). This material is based upon work supported by the National Center for Atmospheric Research, which is a major facility sponsored by the National Science Foundation under cooperative agreement no. 1852977.Peer ReviewedPostprint (published version

Chemistry Across Multiple Phases (CAMP) version 1.0: an integrated multiphase chemistry model

A flexible treatment for gas- and aerosol-phase chemical processes has been developed for models of diverse scale, from box models up to global models. At the core of this novel framework is an “abstracted aerosol representation” that allows a given chemical mechanism to be solved in atmospheric models with different aerosol representations (e.g., sectional, modal, or particle-resolved). This is accomplished by treating aerosols as a collection of condensed phases that are implemented according to the aerosol representation of the host model. The framework also allows multiple chemical processes (e.g., gas- and aerosol-phase chemical reactions, emissions, deposition, photolysis, and mass transfer) to be solved simultaneously as a single system. The flexibility of the model is achieved by (1) using an object-oriented design that facilitates extensibility to new types of chemical processes and to new ways of representing aerosol systems, (2) runtime model configuration using JSON input files that permits making changes to any part of the chemical mechanism without recompiling the model (this widely used, human-readable format allows entire gas- and aerosol-phase chemical mechanisms to be described with as much complexity as necessary), and (3) automated comprehensive testing that ensures stability of the code as new functionality is introduced. Together, these design choices enable users to build a customized multiphase mechanism without having to handle preprocessors, solvers, or compilers. Removing these hurdles makes this type of modeling accessible to a much wider community, including modelers, experimentalists, and educators. This new treatment compiles as a stand-alone library and has been deployed in the particle-resolved PartMC model and in the Multiscale Online AtmospheRe CHemistry (MONARCH) chemical weather prediction system for use at regional and global scales. Results from the initial deployment to box models of different complexity and MONARCH will be discussed, along with future extension to more complex gas–aerosol systems and the integration of GPU-based solvers.Matthew L. Dawson has received funding from the European Union's Horizon 2020 research and innovation program under Marie Skłodowska-Curie grant agreement no. 747048. Matthew L. Dawson, Oriol Jorba, and Christian Guzman have been supported by the Ministerio de Ciencia, Innovación y Universidades (grant no. RTI2018-099894-BI00). Christian Guzman acknowledges funding from the AXA Research Fund. Nicole Riemer, Matthew West, and Jeffrey H. Curtis acknowledge funding from the National Science Foundation (grant no. AGS 19-41110). This material is based upon work supported by the National Center for Atmospheric Research, which is a major facility sponsored by the National Science Foundation under cooperative agreement no. 1852977.Peer ReviewedPostprint (published version