scholarly journals The Atmospheric Chemistry and Canopy Exchange Simulation System (ACCESS): model description and application to a temperate deciduous forest canopy

2012 ◽  
Vol 12 (9) ◽  
pp. 24765-24820 ◽  
Author(s):  
R. D. Saylor

Abstract. Forest canopies are primary emission sources of biogenic volatile organic compounds (BVOCs) and have the potential to significantly influence the formation and distribution of secondary organic aerosol (SOA) mass. Biogenically-derived SOA formed as a result of emissions from the widespread forests across the globe may affect air quality in populated areas, degrade atmospheric visibility, and affect climate through direct and indirect forcings. In an effort to better understand the formation of SOA mass from forest emissions, a 1-D column model of the physical and chemical processes occurring within and just above a vegetative canopy has been created. This model, the Atmospheric Chemistry and Canopy Exchange Simulation System (ACCESS), includes processes accounting for the emission of BVOCs from the canopy, turbulent vertical transport within and above the canopy and throughout the height of the planetary boundary layer (PBL), near-explicit representation of chemical transformations, mixing with the background atmosphere and bi-directional exchange between the atmosphere and canopy and the atmosphere and forest floor. The model formulation of ACCESS is described in detail and results are presented for an initial application of the modeling system to Walker Branch Watershed, an isoprene-emission-dominated forest canopy in the Southeastern United States which has been the focal point for previous chemical and micrometeorological studies. Model results of isoprene profiles and fluxes are found to be consistent with previous measurements made at the simulated site and with other measurements made in and above mixed deciduous forests in the Southeastern United States. Sensitivity experiments exploring how canopy concentrations and fluxes of gas-phase precursors of SOA are affected by background anthropogenic nitrogen oxides suggest potentially significant non-linearities in the chemical and physical system of the canopy which may have an impact on the relative magnitude of SOA formed through aqueous- versus gas-phase pathways as a function of anthropogenic influence.

2013 ◽  
Vol 13 (2) ◽  
pp. 693-715 ◽  
Author(s):  
R. D. Saylor

Abstract. Forest canopies are primary emission sources of biogenic volatile organic compounds (BVOCs) and have the potential to significantly influence the formation and distribution of secondary organic aerosol (SOA) mass. Biogenically-derived SOA formed as a result of emissions from the widespread forests across the globe may affect air quality in populated areas, degrade atmospheric visibility, and affect climate through direct and indirect forcings. In an effort to better understand the formation of SOA mass from forest emissions, a 1-D column model of the multiphase physical and chemical processes occurring within and just above a vegetative canopy is being developed. An initial, gas-phase-only version of this model, the Atmospheric Chemistry and Canopy Exchange Simulation System (ACCESS), includes processes accounting for the emission of BVOCs from the canopy, turbulent vertical transport within and above the canopy and throughout the height of the planetary boundary layer (PBL), near-explicit representation of chemical transformations, mixing with the background atmosphere and bi-directional exchange between the atmosphere and canopy and the atmosphere and forest floor. The model formulation of ACCESS is described in detail and results are presented for an initial application of the modeling system to Walker Branch Watershed, an isoprene-emission-dominated forest canopy in the southeastern United States which has been the focal point for previous chemical and micrometeorological studies. Model results of isoprene profiles and fluxes are found to be consistent with previous measurements made at the simulated site and with other measurements made in and above mixed deciduous forests in the southeastern United States. Sensitivity experiments are presented which explore how canopy concentrations and fluxes of gas-phase precursors of SOA are affected by background anthropogenic nitrogen oxides (NOx). Results from these experiments suggest that the level of ambient NOx influences the pathways by which SOA is formed by affecting the relative magnitudes and fluxes of isoprene oxidation products emitted from the canopy. Future versions of the ACCESS model are planned to be multiphase, including gas- and aerosol-phase chemical and physical processes, to more fully explore these preliminary results.


2016 ◽  
Author(s):  
Kirsti Ashworth ◽  
Serena H. Chung ◽  
Karena A. McKinney ◽  
Ying Liu ◽  
Bill J. Munger ◽  
...  

Abstract. The FORCAsT canopy exchange model was used to investigate the underlying mechanisms governing foliage emissions of methanol and acetaldehyde, two short chain oxygenated volatile organic compounds ubiquitous in the troposphere and known to have strong biogenic sources, at a northern mid-latitude forest site. The explicit representation of the vegetation canopy within the model allowed us to test the hypothesis that stomatal conductance regulates emissions of these compounds to an extent that its influence is observable at the ecosystem-scale, a process not currently considered in regional or global scale atmospheric chemistry models. We found that FORCAsT could only reproduce the magnitude and diurnal profiles of methanol and acetaldehyde fluxes measured at the top of the forest canopy at Harvard Forest if light-dependent emissions were introduced to the model. With the inclusion of such emissions FORCAsT was able to successfully simulate the observed bi-directional exchange of methanol and acetaldehyde. Although we found evidence that stomatal conductance influences methanol fluxes and concentrations at scales beyond the leaf-level, particularly at dawn and dusk, we were able to adequately capture ecosystem exchange without the addition of stomatal control to the standard parameterisations of foliage emissions, suggesting that ecosystem fluxes can be well enough represented by the emissions models currently used.


2017 ◽  
Author(s):  
Havala O. T. Pye ◽  
Andreas Zuend ◽  
Juliane L. Fry ◽  
Gabriel Isaacman-VanWertz ◽  
Shannon L. Capps ◽  
...  

Abstract. Several models were used to describe the partitioning of ammonia, water, and organic compounds between the gas and particle phase for conditions in the southeastern United States during summer 2013. Existing equilibrium models and frameworks were found to be sufficient although additional improvements in terms of estimating pure-species vapor pressures are needed. Thermodynamic model predictions were consistent, to first order, with a molar ratio of ammonium to sulfate of approximately 1.6 to 1.8 (Ratio of ammonium to 2 × sulfate, RN/2S ≈ 0.8 to 0.9) with approximately 70 % of total ammonia and ammonium (NHx) in the particle. Southeastern Aerosol Research and Characterization (SEARCH) network gas and aerosol and Southern Oxidant and Aerosol Study (SOAS) Monitor for Aerosols and Gases in Air (MARGA) aerosol measurements were consistent with these conditions. CMAQv5.2 regional chemical transport model predictions did not reflect these conditions due to biases in the nonvolatile cations that resulted from either overestimated emissions and/or underestimated mixing. In addition, gas-phase ammonia was overestimated in the CMAQ model leading to an even lower fraction of total ammonia in the particle. Chemical Speciation Network (CSN) and Aerosol Mass Spectrometer (AMS) measurements indicated less ammonium per sulfate than SEARCH and MARGA measurements and were inconsistent with thermodynamic model predictions. Organic compounds were predicted to be present to some extent in the same phase as inorganic constituents, modifying their activity and resulting in a decrease in [H+]air (H+ in μg m−3 air), increase in ammonia partitioning to the gas phase, and increase in pH compared to complete organic vs. inorganic liquid-liquid phase separation. In addition, accounting for non-ideal mixing modified the pH such that a fully interactive inorganic-organic system had a pH roughly 0.7 units higher than predicted by traditional methods (pH = 1.5 vs. 0.7). Particle-phase interactions of organic and inorganic compounds were found to increase partitioning towards the particle phase (vs. gas phase) for highly oxygenated (O : C ≥ 0.6) compounds including several isoprene-derived tracers as well as levoglucosan, but decrease particle-phase partitioning for low O : C, monoterpene-derived species.


2016 ◽  
Vol 16 (24) ◽  
pp. 15461-15484 ◽  
Author(s):  
Kirsti Ashworth ◽  
Serena H. Chung ◽  
Karena A. McKinney ◽  
Ying Liu ◽  
J. William Munger ◽  
...  

Abstract. The FORCAsT canopy exchange model was used to investigate the underlying mechanisms governing foliage emissions of methanol and acetaldehyde, two short chain oxygenated volatile organic compounds ubiquitous in the troposphere and known to have strong biogenic sources, at a northern mid-latitude forest site. The explicit representation of the vegetation canopy within the model allowed us to test the hypothesis that stomatal conductance regulates emissions of these compounds to an extent that its influence is observable at the ecosystem scale, a process not currently considered in regional- or global-scale atmospheric chemistry models.We found that FORCAsT could only reproduce the magnitude and diurnal profiles of methanol and acetaldehyde fluxes measured at the top of the forest canopy at Harvard Forest if light-dependent emissions were introduced to the model. With the inclusion of such emissions, FORCAsT was able to successfully simulate the observed bidirectional exchange of methanol and acetaldehyde. Although we found evidence that stomatal conductance influences methanol fluxes and concentrations at scales beyond the leaf level, particularly at dawn and dusk, we were able to adequately capture ecosystem exchange without the addition of stomatal control to the standard parameterisations of foliage emissions, suggesting that ecosystem fluxes can be well enough represented by the emissions models currently used.


2019 ◽  
Author(s):  
Jorge Noguera

This study was conducted to determine the effectiveness of a novel mind perception manipulation. Mind perception is currently theorized to be an essential aspect of a number of human social psychological processes. Thus, a successful manipulation would allow for the causal study of those processes. This manipulation was created in an attempt to explore the downstream impact of mind perception on the endorsement of conspiracy theories. Conspiracy theories are steadily becoming more and more prominent in social discourse. Endorsement of conspiracy theories are beginning to show real world ramifications such as a danger to human health (e.g., in the anti-vaccination movement). A sample of college students (valid N = 53) from a large rural institution in the southeastern United States participated for course credit. These participants completed a mind perception pretest, were randomly assigned to either the manipulation in question (in which participants are asked to consider the ‘mind’ of several targets and write their thoughts about them) or the control condition, and then they completed a posttest. The mixed ANOVA revealed that the interaction term between Time and Condition was not significant. Because the manipulation did not work, other analyses were aborted, in accord with the pre-registration. My Discussion focuses on the procedures and potential shortcomings of this manipulation, in an effort to lay the groundwork for a successful one.


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