scholarly journals Modelling bidirectional fluxes of methanol and acetaldehyde with the FORCAsT canopy exchange model

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.

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.


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.


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.


2004 ◽  
Vol 4 (2) ◽  
pp. 1291-1310 ◽  
Author(s):  
C. R. Trostdorf ◽  
L. V. Gatti ◽  
A. Yamazaki ◽  
M. J. Potosnak ◽  
A. Guenther ◽  
...  

Abstract. Tropical forests are an important global source of volatile organic compounds (VOCs) and other atmospheric trace gases. The high biodiversity in tropical rainforests complicates the extrapolation of biogenic volatile organic compound (BVOC) emissions from leaf-level measurements to landscape and regional or global scales. In Amazônia, a significant fraction of the carbon emitted from the biosphere to the atmosphere is emitted in the form of BVOCs, and the knowledge of these emissions is important to our understanding of tropical and global atmospheric chemistry and carbon cycling. As part of the Large scale Biosphere-atmosphere experiment in Amazônia (LBA). VOC concentrations were measured at two sites near Santarém, Para State, Brazil. The two sites are located in the National Forest of Tapajós, the first corresponding to primary forest and the second to a forest, that was selectively logged. The samples were collected simultaneously at heights of 65 and 55 m (20 and 10 m above forest canopy, respectively). The average isoprene mixing ratio was 2.2–2.5 ppb at the two sites and the standard deviations within a site ranged from 1 to 1.2 ppb. A strong seasonality of isoprene mixing ratio was observed and associated with the wet and dry seasons. The lowest mixing ratios were found during the transition between the wet to dry season, while at the start of the biomass burning season the mixing ratios increase. A qualitative analysis of a one dimensional model demonstrates that the seasonal cycle in concentrations reflects changes in isoprene production by the ecosystem, not changes in boundary layer dynamics or chemistry. The magnitude of the cycle indicates that the physiological capacity of the ecosystem to emit isoprene may depend on water availability although phenological changes could also contribute to the observed variations. A simple 1-D model that assumes mean daytime isoprene fluxes of 1.5 mg m−2h−1 and 0.9 mg m−2h−1 scaled by an algorithm depending on precipitation at the primary forest and selectively logged sites, respectively, is able to reproduce the observed vertical gradients.


2009 ◽  
Vol 9 (5) ◽  
pp. 18899-18963 ◽  
Author(s):  
C. N. Hewitt ◽  
J. Lee ◽  
M. P. Barkley ◽  
N. Carslaw ◽  
N. A. Chappell ◽  
...  

Abstract. In April–July 2008, intensive measurements were made of atmospheric composition and chemistry in Sabah, Malaysia, as part of the "Oxidant and particle photochemical processes above a South-East Asian tropical rain forest" (OP3) project. Fluxes and concentrations of trace gases and particles were made from and above the rain forest canopy at the Bukit Atur Global Atmosphere Watch station and at the nearby Sabahmas oil palm plantation, using both ground-based and airborne measurements. Here, the measurement and modelling strategies used, the characteristics of the sites and an overview of data obtained are described. Composition measurements show that the rainforest site was not impacted by significant sources of anthropogenic pollution, and this is confirmed by satellite retrievals of NO2 and HCHO. The dominant modulators of atmospheric chemistry at the rain forest site were therefore emissions of BVOCs and soil emissions of reactive nitrogen oxides. At the observed BVOC:NOx volume mixing ratio (~104 pptv/pptv), current chemical models suggest that daytime maximum OH concentrations should be ca. 105 radicals cm−3, but observed OH concentrations were an order of magnitude greater than this. We confirm, therefore, previous measurements which suggest that an unexplained source of OH must exist above tropical forests and continue to interrogate the data to find explanations for this.


2020 ◽  
Vol 20 (19) ◽  
pp. 11287-11304
Author(s):  
Wei Wang ◽  
Laurens Ganzeveld ◽  
Samuel Rossabi ◽  
Jacques Hueber ◽  
Detlev Helmig

Abstract. During the Program for Research on Oxidants: PHotochemistry, Emissions, and Transport (PROPHET) campaign from 21 July to 3 August 2016, field experiments on leaf-level trace gas exchange of nitric oxide (NO), nitrogen dioxide (NO2), and ozone (O3) were conducted for the first time on the native American tree species Pinus strobus (eastern white pine), Acer rubrum (red maple), Populus grandidentata (bigtooth aspen), and Quercus rubra (red oak) in a temperate hardwood forest in Michigan, USA. We measured the leaf-level trace gas exchange rates and investigated the existence of an NO2 compensation point, hypothesized based on a comparison of a previously observed average diurnal cycle of NOx (NO2+NO) concentrations with that simulated using a multi-layer canopy exchange model. Known amounts of trace gases were introduced into a tree branch enclosure and a paired blank reference enclosure. The trace gas concentrations before and after the enclosures were measured, as well as the enclosed leaf area (single-sided) and gas flow rate to obtain the trace gas fluxes with respect to leaf surface. There was no detectable NO uptake for all tree types. The foliar NO2 and O3 uptake largely followed a diurnal cycle, correlating with that of the leaf stomatal conductance. NO2 and O3 fluxes were driven by their concentration gradient from ambient to leaf internal space. The NO2 loss rate at the leaf surface, equivalently the foliar NO2 deposition velocity toward the leaf surface, ranged from 0 to 3.6 mm s−1 for bigtooth aspen and from 0 to 0.76 mm s−1 for red oak, both of which are ∼90 % of the expected values based on the stomatal conductance of water. The deposition velocities for red maple and white pine ranged from 0.3 to 1.6 and from 0.01 to 1.1 mm s−1, respectively, and were lower than predicted from the stomatal conductance, implying a mesophyll resistance to the uptake. Additionally, for white pine, the extrapolated velocity at zero stomatal conductance was 0.4±0.08 mm s−1, indicating a non-stomatal uptake pathway. The NO2 compensation point was ≤60 ppt for all four tree species and indistinguishable from zero at the 95 % confidence level. This agrees with recent reports for several European and California tree species but contradicts some earlier experimental results where the compensation points were found to be on the order of 1 ppb or higher. Given that the sampled tree types represent 80 %–90 % of the total leaf area at this site, these results negate the previously hypothesized important role of a leaf-scale NO2 compensation point. Consequently, to reconcile these findings, further detailed comparisons between the observed and simulated in- and above-canopy NOx concentrations and the leaf- and canopy-scale NOx fluxes, using the multi-layer canopy exchange model with consideration of the leaf-scale NOx deposition velocities as well as stomatal conductances reported here, are recommended.


1984 ◽  
Vol 21 (2) ◽  
pp. 643 ◽  
Author(s):  
J. Roberts ◽  
J. S. Wallace ◽  
R. M. Pitman

2019 ◽  
Author(s):  
Jarmo Mäkelä ◽  
Jürgen Knauer ◽  
Mika Aurela ◽  
Andrew Black ◽  
Martin Heimann ◽  
...  

Abstract. We calibrated the JSBACH model with six different stomatal conductance formulations using measurements from 10 FLUXNET coniferous evergreen sites in the Boreal zone. The parameter posterior distributions were generated by adaptive population importance sampler and the optimal values by a simple stochastic optimisation algorithm. The observations used to constrain the model are evapotranspiration (ET) and gross primary production (GPP). We identified the key parameters in the calibration process. These parameters control the soil moisture stress function and the overall rate of carbon fixation. We were able to improve the coefficient of determination and the model bias with all stomatal conductance formulations. There was no clear candidate for the best stomatal conductance model, although certain versions produced better estimates depending on the examined variable (ET, GPP) and the used metric. We were also able to significantly enhance the model behaviour during a drought event in a Finnish Scots pine forest site. The JSBACH model was also modified to use a delayed effect of temperature for photosynthetic activity. This modification enabled the model to correctly time and replicate the springtime increase in GPP (and ET) for conifers throughout the measurements sites used in this study.


2015 ◽  
Vol 15 (13) ◽  
pp. 7413-7427 ◽  
Author(s):  
G. Wohlfahrt ◽  
C. Amelynck ◽  
C. Ammann ◽  
A. Arneth ◽  
I. Bamberger ◽  
...  

Abstract. Methanol is the second most abundant volatile organic compound in the troposphere and plays a significant role in atmospheric chemistry. While there is consensus about the dominant role of living plants as the major source and the reaction with OH as the major sink of methanol, global methanol budgets diverge considerably in terms of source/sink estimates, reflecting uncertainties in the approaches used to model and the empirical data used to separately constrain these terms. Here we compiled micrometeorological methanol flux data from eight different study sites and reviewed the corresponding literature in order to provide a first cross-site synthesis of the terrestrial ecosystem-scale methanol exchange and present an independent data-driven view of the land–atmosphere methanol exchange. Our study shows that the controls of plant growth on production, and thus the methanol emission magnitude, as well as stomatal conductance on the hourly methanol emission variability, established at the leaf level, hold across sites at the ecosystem level. Unequivocal evidence for bi-directional methanol exchange at the ecosystem scale is presented. Deposition, which at some sites even exceeds methanol emissions, represents an emerging feature of ecosystem-scale measurements and is likely related to environmental factors favouring the formation of surface wetness. Methanol may adsorb to or dissolve in this surface water and eventually be chemically or biologically removed from it. Management activities in agriculture and forestry are shown to increase local methanol emission by orders of magnitude; however, they are neglected at present in global budgets. While contemporary net land methanol budgets are overall consistent with the grand mean of the micrometeorological methanol flux measurements, we caution that the present approach of simulating methanol emission and deposition separately is prone to opposing systematic errors and does not allow for full advantage to be taken of the rich information content of micrometeorological flux measurements.


Sign in / Sign up

Export Citation Format

Share Document