Nitrogen deposition in tropical forests from deforestation and savanna fires

Running title: Fire effects on tropical N fluxes

Yang Chen, Department of Earth System Science, University of California, Irvine, CA 92697, USA James T. Randerson, Department of Earth System Science, University of California, Irvine, CA 92697, USA Guido R. van der Werf, Faculty of Earth and Life Sciences, VU University, 1081HV Amsterdam, Netherlands Douglas C. Morton, NASA Goddard Space Flight Center, Biospheric Sciences Branch, Code 614.4, Greenbelt, Maryland USA 20771 Prasad S. Kasibhatla, Nicholas School of the Environment, Duke University, Durham, NC 27708, USA

Kewords: atmospheric transport, pyro-denitrification, nitrogen limitation, Hadley circulation, tropical biomes, the global carbon cycle, and biomass burning Category of article: Primary Research Article

Corresponding author Yang Chen Email: yang.chen@uci.edu Phone: 1-949-824-0597 Department of Earth System Science, University of California, Irvine, CA 92697

Manuscript prepared for Global Change Biology June 11, 2009

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Abstract
Tropical forests account for nearly half of global net primary production (NPP) and may contribute substantially to contemporary and future land carbon (C) sinks. We used satellite-derived estimates of global fire emissions and a chemical transport model to estimate atmospheric nitrogen (N) fluxes from deforestation and savanna fires in tropical ecosystems. N emissions and deposition led to a substantial net transport of N equatorward, from savannas and areas undergoing deforestation to tropical forests. On average, N emissions from fires were equivalent to approximately 28% of biological N fixation (BNF) in savannas (4.8 kg N ha-1 yr-1) and 38% of BNF from ecosystems at the deforestation frontier (9.1 kg N ha-1 yr-1). N deposition occurred in interior tropical forests at a rate equivalent to 4% of their BNF (1.1 kg N ha-1 yr-1). This percentage was highest for African tropical forests in the Congo Basin (16%; 3.7 kg N ha-1 yr-1) owing to equatorward transport from northern and southern savannas. These results suggest that land use change, including deforestation fires, may be enhancing nutrient availability and carbon sequestration in nearby tropical forest ecosystems.

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INTRODUCTION
Nitrogen (N) is an essential element in Earth's atmosphere, biosphere, and hydrosphere (Galloway et al., 2003). The majority of N in the atmosphere is N2, which is biologically unavailable to most organisms. N2 must be converted to reactive N (Nr), which includes inorganic oxidized forms (e.g., NO, NO2, and HNO3), inorganic reduced forms (NH3 and NH4+), and organic forms (e.g., amino acids and urea), prior to its use by microbes and plants. N2 to Nr conversion (N fixation) occurs during electrical discharges in lightning and by some bacteria and algae via a process known as biological nitrogen fixation (BNF) (Cleveland et al., 1999). Humans have more than doubled the flux of N2 to Nr through fossil fuel use, industrial N fertilizer production, and cultivation of N fixing leguminous crops (Vitousek et al., 1997; Smil, 1999; Galloway et al., 2004, 2008). Atmospheric transport and deposition of N emissions substantially changes N availability in terrestrial ecosystems. Major effects of N deposition have been documented in terrestrial and marine ecosystems (e.g., Fenn et al., 2003). Since most terrestrial ecosystems are N-limited, N addition to these ecosystems stimulates net primary production (NPP) (LeBauer & Treseder, 2008) and may enhance carbon (C) storage by this mechanism (e.g., Holland et al., 1997, Reay et al., 2008). However, chronic N enrichment may lead to loss of C by increasing decomposition in organic soils (Mack et al., 2004) or in soil carbon components that have decadal turnover times (Neff et al., 2002). In some ecosystems, N addition also reduces microbial biomass and decreases soil respiration (Treseder, 2008). N deposition can also influence ecosystem function by means of acidification, eutrophication (Rabalais, 2002), and loss of species diversity (Wilson and Tilman, 2002; Suding et al., 2005; Phoenix et al.,

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2006). Much of our knowledge of the N cycle and the consequences of N enrichment are from temperate ecosystems, where industrial and agricultural modifications of N availability are substantial. Tropical ecosystems respond in different ways to perturbations in N cycling (Matson et al., 1999; Davidson et al., 2004) and important uncertainties remain with respect to our understanding of N deposition, fixation, and loss pathways in these ecosystems. With implementation of stricter air quality standards, N emission and deposition are likely to slow down in temperate regions, particularly in developed countries (Lamarque et al., 2005; Dentener et al., 2006). In contrast, N emission and deposition in tropical and subtropical regions should increase (Galloway et al., 1994). Since tropical ecosystems account nearly half of global NPP (Field et al., 1998) and may contribute substantially to contemporary and future land C sinks (Friedlingstein et al., 2006; Stephens et al., 2007), it is imperative to identify and quantify the consequences of changing levels of N deposition and N cycling in tropical ecosystems. Fires in savanna and at the deforestation frontier are a major source of air pollution in the tropics (Crutzen and Andreae, 1990). Nitrogen oxide (NO) and ammonia (NH3) are the primary Nr gases emitted from these fires. They are converted to other Nr gases and to particulate species (NO3-, NH4+, and organic aerosols) by means of multiple reaction pathways (Crutzen and Andreae, 1990; Atkinson, 2000). The ultimate fate of Nr in the atmosphere is removal by wet and dry deposition. Gas and aerosol components of dry deposition are important in many regions (Dentener et al., 2006). Regional variations in emissions and atmospheric transport of Nr have the potential to create strong gradients of

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2001. We estimated N2 emissions from biomass burning using data derived from a chamber burning experiment (Kuhlbusch et al. 1990. van der Werf et al.. We explored the loss of N by emissions from biomass burning and the gain of Nr by deposition from the atmosphere. 5 .. 1999. The N2 emission represents a net loss of N from the biosphere– contrasting with Nr fluxes that instead lead to redistribution of Nr across different ecosystems.. In this study. which combines satellite observations of burned area (Giglio et al. The transport and deposition of N were simulated by using the GEOS-Chem global chemical transport model (CTM) (Bey et al. We performed 10 years (1997–2006) of global-scale simulations but focus our analysis and discussion on tropical ecosystems. 2001). These fluxes were then compared with terrestrial and marine BNF fluxes (Cleveland et al. 2002). 1991).N deposition across both terrestrial and ocean ecosystems.. We estimated fire emissions using the Global Fire Emission Database version 2 (GFEDv2. Lee et al. 2006).. as some is retained within the ecosystem in combusted residues (approximately 20%) and the remainder (another 30–40%) is transformed directly into N2 during the combustion processes (Lobert et al. Emissions of NO and NH3 probably account for only 40-50% of the N present in fuels prior to combustion. 2006) and a biogeochemical model constrained by other satellite data to estimate fuel loads. We validated some of our modeled fluxes by comparing our results with published observations of N deposition.. Kuhlbusch et al... 1991). Deutsch et al.. We also estimated the net N flux from fire emissions in different tropical ecosystems. we assessed the contribution of fires to N cycling in tropical ecosystems.

were obtained from Andreae and Merlet (2001). required a small negative adjustment (from 0-22% depending on atmospheric inversion approach) to match Measurements of Pollution in the Troposphere (MOPITT) observations during 2000-2006 (van der Werf et al. GFEDv2 CO emissions in equatorial Asia. Fuel loads were estimated using the Carnegie-Ames-Stanford-Approach (CASA) biogeochemical model constrained by additional satellite observations of fractional tree cover and the fraction of absorbed photosynthetically active radiation by plant canopies (van der Werf et al.. 2008). 2006). combustion completeness (CC).79 with observations from NOAA Global Monitoring Division (GMD) stations in the Northern Hemisphere 6 .. Comparison with atmospheric carbon monoxide (CO) observations provides some validation of carbon emissions. CO anomalies from GFEDv2 in the GEOS-CHEM model had a mean correlation of 0.METHODS Nr emissions from biomass burning The GFEDv2 product consists of 1°×1° gridded monthly burned area (BA). Burned area was derived using Moderate Resolution Imaging Spectroradiometer (MODIS) active fire and burned area datasets as described by Giglio et al.. fuel loads (FL). Emission factors. and emissions factors (EMFs) for different gas and aerosol species (van der Werf et al. Emission rates (E) for each gaseous N species were calculated by applying EMFs to fire-emitted carbon fluxes from CASA: E = EMF × BA × FL × CC (1) Organic dry matter (DM) in the fuel was assumed to be comprised of 45% carbon. defined as the emission of species (g) per 1 kg burned DM. 2006). 2003. (2006). for example.

. Nr to N2 conversion during biomass burning A large gap has been observed in the N balance between its content in the fuel and the sum of measured N in gaseous emissions and what remains after combustion in the ash (Lobert et al.59 with GMD stations in the Southern Hemisphere (Kai et al.g.09. Kuhlbusch et al. (1991) showed that the missing N is mostly molecular N (N2)..86 and 1. van der Werf et al. In our model simulations and calculations.g. CO/CO2 emission ratio 7 . This experiment also showed that N2 is formed primarily during the flaming stage and thus the total amount of N2 production (as a fraction of fuel N) depends on fire intensity. for northern and southern hemispheres. they are of sufficient quality to study the impact of fire-emitted species on atmospheric composition. Giglio et al. 2006) and total carbon emissions (e. By burning different biomass materials in a stainless steel chamber. which accounts for approximately one third of fuel N..and 0. 2001). The low bias we expect from neglecting the remaining Nr emissions (e. Similarly. Nr can be emitted into the atmosphere in different chemical forms and physical phases.. N2O.g. 2008). 1990). we used the sum of gaseous NOx and NH3 emissions to represent total Nr emissions from biomass burning. the ratio of modeled to observed standard deviations of CO anomalies from GMD was 0.. HCN. These results indicate that while emissions estimates are still uncertain. respectively.. NOx and NH3 account for the majority (greater than 90%) of Nr emissions from biomass burning (Andreae and Merlet. and acetonitrile) is small compared with uncertainties associated with our estimates of burned area (e. 2009)..

aircraft.. In this study.01 hPa. fossil fuel. 1998). and extratropical forest fires using the emission factors of CO and CO2 listed in Table 1 of Andreae and Merlet (2001). For each grid cell. Emission sources of N include NOx from lightning. Model simulations of N transport and deposition We used the GEOS-Chem model to calculate the transport.5° horizontal resolution and 30 vertical layers between the surface and 0. soil and fertilizer. and 8 . and NH3 from biofuel. fossil fuel. transformation. (1991) measurements showed that the N2-N to Nr-N ratio of fire emissions was inversely related to its CO/CO2 ratio (see Fig.serves as a powerful indicator for the relative extent of flaming combustion and smoldering combustion. tropical forest fires. 2001) driven by assimilated meteorological observations from the Goddard Earth Observing System (GEOS) of the NASA Global Modeling and Assimilation Office (GMAO). the GFEDv2 Nr emission rate was scaled by this ratio to approximate the fire emission rate of N2. GEOS-Chem is a global 3-D CTM (Bey et al. The N2-N to Nr-N ratio derived from this relationship was used to estimate global N2 emissions from biomass burning. we used version 08-01-01 of the model with 2°×2. and deposition of biomass burning emitted N species.. biomass burning.5°(longitude) vegetation map of these three types (Andreae and Merlet. Analysis of the Kuhlbusch et al. biomass burning. A 2°(latitude) × 2. we estimated the CO/CO2 ratio for three different fire types: savanna and grassland fires. The GEOS-Chem model includes a detailed description of tropospheric O3-NOx-hydrocarbon chemistry (Wang et al. In this study. 2001) was used to derive the global gridded N2-N to Nr-N ratio. S1 in Supporting Information). biofuel.

After a three-month spin-up period with the same initial conditions. We performed GEOS-Chem full chemistry simulations over a 10-year period (1997-2006) using the GFEDv2 inventory.. (2004) argued that the true N fixation rate lies at the lower end of this 9 . and upper-bound) between BNF and evapotranspiration (ET) in terrestrial ecosystems. peroxyacyl nitrate (PAN). soils. The difference between these two simulations represents the effect of biomass burning emissions on N transport and deposition. and another without these emissions. N2O5. vegetation. and wild animals). N tracers are present in gas phase (e. N on sulfate.g. We recorded monthly mean deposition rates for each N species through dry and wet deposition.. (1999) reviewed published studies and generated three linear regressions (conservative. Total deposition rate of N from biomass burning was then calculated for each 2°×2. and NH3) or aerosol phase (NH4+. These tracers are transported by meteorology-driven advection and convection processes. Biological N fixation Cleveland et al. and N on sea salt). Galloway et al.5° model grid cell. HNO3. which resolves the interannual variability of biomass burning emissions. 2001). central.g. and finally removed by the action of precipitation (wet deposition) or by contact with surface or vegetation (dry deposition).. N emissions from other sources were obtained from climatological inventories which represent contemporary (circa 2000) emissions.natural sources (e. Wet deposition included convective and large-scale components (Liu et al. two sets of simulations were conducted: one with biomass burning emissions prescribed from GFEDv2. NOx.

. Large uncertainty remains in the estimation of regional marine N fixation (Mahaffey et al.. Due to a dearth of data for other regions.. The global ET map we used was developed using satellite data and a biometeorological approach by Fisher et al. Estimates of global ocean BNF range from 60 to 200 Tg N yr-1 (Duce et al.. due to the inherent biases noted in plot-scale studies. (2008). 2005).range. we used reported estimates of BNF rates over tropical Atlantic (Lee et al. In this study. In this study. 2001). we therefore used the mean of central and conservative regressions between BNF and ET from Cleveland et al. (1999) to estimate N fixation rates over land. 2008). 2002) and Pacific (Deutsch et al. 10 . we assumed that the mean of these two rates represented the N fixation rate over other tropical oceans.

For locations that had measurements only during 1996. the model simulation corresponded reasonably well to wet and dry deposition observations at non-urban sites (Fig. The model somewhat underestimated NO3-N wet deposition and overestimated NH4-N dry deposition. Based on the original data. 2006). The location and time period of these measurements. Dentener et al. we reported wet and dry deposition rates from 26 non-urban stations. We differentiated urban and non-urban observations according to the description of the site in the original literature or the proximity of the measurement station to an urban center. 11 . which were sampled in grid cells corresponding to observations during the month when observations were available. we compared the deposition rates with our 10-year (1997–2006) mean model results. Altogether.. This agreement was similar to previous comparisons of N deposition between models and observations (Lamarque et al. We compared these observations with modeled deposition fluxes..RESULTS Validation of wet and dry deposition Relative to Northern Hemisphere industrial regions. Here we compiled wet and dry N deposition measurements in tropical regions published in recent years. are summarized in Table S1. About 75% of the wet deposition rates and 80% of the dry deposition rates agreed within ±50% with the observations. We only considered observations from 1996 to 2006 to ensure overlap with the period of our satellite-derived fire emissions time series. Overall. as well observed and modeled deposition rates. 2005. fewer N deposition measurements exist for tropical land and ocean regions. 1). we calculated wet and dry deposition rates for total oxidized N (NO3-N) and reduced N (NH4-N) with units of kg N ha-1 yr-1.

8 kg N ha-1 yr-1) in tropical forests.7 kg N ha-1 yr-1). Losses directly to N2 accounted for about half of the total N emissions flux. with these two biomes accounting for 67% of global fire N emissions (Fig.9 kg N ha-1 yr-1). as well as in deforestation regions (See Fig. 1). In contrast to non-urban sites.with maxima on the perimeter of the Congo basin in Africa (up to 9. 2a and Table 1). and Paraguay in South America (up to 5. S3). Deposition rates were highest near source regions .5° grid cells in the model.5 kg N ha-1 yr-1) in savannas and 5.4 Tg N yr-1 (6. 1. S2) in South America and Southeast Asia. High emission rates occurred in African savannas.3 Tg N yr-1 (3. as indicated by the r values shown in Fig. This fraction was slightly higher for savannas than for tropical forests because of more complete combustion (and lower CO/CO2 ratios in savannas). N deposition rates from biomass burning Fire emissions represented a considerable fraction of N deposition in the tropics (See Fig.Simulations were more strongly correlated with measurements for dry deposition than for wet deposition. so they were not included in our linear regressions. We note most of these urban measurement sites were located in Southeast Asia.3 12 . which were likely affected by nearby fossil fuel emissions (Fig. Gross N emissions from fires Emissions of Nr and N2 by fires were 10. and across the Brazilian state of Mato Grosso. in southern Borneo in equatorial Asia (up to 9. Urban data were generally not representative of the 2°×2. eastern Bolivia. the model was generally biased low relative to the high urban data.

g. Changes in N surface budgets caused by fire emissions The emission and deposition of N from fires led to a net loss of N from the terrestrial biosphere and a redistribution of N among ecosystems. 2c. causing changes in species composition in ecosystems such as heathlands (van der Berg et al. Reduced N. for example. S2). The relative importance of wet deposition as an atmospheric loss pathway increased towards the end of the fire season on all three continents (Fig.kg N ha-1 yr-1) (Fig. 3). Net gains at a 13 . 2b). Total wet deposition was comparable to total dry deposition across the tropics. 2008) and peatlands (Paulissen et al. although regionally the relative importance of these two pathways varied. These results imply that undisturbed forest and savanna ecosystems in these regions (e. Savanna ecosystems in Africa and South America and tropical deforestation frontiers in all three regions experienced a net loss of N (Figs. 2004). 3). Wet deposition accounted for a larger fraction of total deposition in Southeast Asia (57%) and Northern Hemisphere (NH) Africa (55%) than in South America (46%) or Southern Hemisphere (SH) Africa (39%).. 1998).. probably as a consequence of increasing precipitation levels. can reduce base cation uptake by plants (de Graaf et al. About 2/3 of the total N wet deposition occurred in the gas phase (NH3 and HNO3). Seasonal variations in N deposition were closely linked with the timing of fire emissions (Fig. Model estimates of the total deposition rate for oxidized N and reduced N were similar.. parks and other protected areas) experience relatively high N deposition from nearby deforestation and savanna fires. Separation of N deposition by its oxidation form is important for assessing N deposition effects on ecosystem function.

where fire return times were lower than on other continents (Giglio et al.46 Tg N yr-1 (3. 2006. In contrast. for example. Expressed as a percentage of BNF. the net atmospheric flux from fires was 0.. the net effect of remote tropical fires was an increase atmospheric deposition. because a larger proportion of fire emissions were associated with deforestation in tropical forests.83 Tg N yr-1 or 2. Net fire losses were equal to approximately 39% of BNF in savanna ecosystems in Africa.7 kg N ha-1 yr-1).19 Tg N yr-1 or 6.. net fire N losses were equal to 28% of BNF (4. 2008). net losses were higher (35%). in the Congo basin) and over the tropical Atlantic Ocean (Fig. In Southeast Asia.regional scale occurred in interior tropical forests and over tropical oceans. Of the directly emitted Nr from African savanna fires. Van der Werf et al.g. tropical forest fires had a net N loss equal to approximately 10% of BNF (2. corresponding to 6. The net loss of N (Nr and N2) from savanna ecosystems was largest in Africa (Table 1). with 55% of Nr emissions remaining within these ecosystems via deposition in nearby areas. net N losses at the deforestation frontier (38%) were 14 . only 53% was returned to savannas via deposition.8 kg N ha-1 yr-1). For savannas across all three continents. Overall. For interior forests in Africa. Most of the remainder was deposited in downwind tropical forests (e. Tropical forests received large N deposition inputs from savanna fires but also lost N through deforestation fires. corresponding to approximately 16% of BNF.7 kg N ha-1 yr-1 in savanna ecosystems (Table S2). In interior tropical forests that were removed from the deforestation frontier (areas with fire emissions below our 500 kg C ha-1 yr-1 threshold).0 kg N ha-1 yr-1). forests at the deforestation frontier in South America and Southeast Asia had a large net N loss at a regional scale from fire emissions.. 2b).

This pattern is consistent with analysis of lidar measurements from Manaus that show long range transport of smoke and dust from Africa (Ansmann et al. S4). Approximately 37% (2. A portion of Nr emitted from savanna fires was deposited back in savannas. Tropical oceans were a large recipient of N from fire emissions.85 Tg N yr-1) of fire-emitted N was deposited over oceans. 2009). in particular. The tropical Atlantic. The N deposition pattern. was similar to that of fire emissions but with a small equatorward shift in peak deposition in the NH. The highest levels of Nr and N2 fire emissions occurred at ~7°N in the northern hemisphere and ~10°S in the southern hemisphere.even higher than in savanna ecosystems. 2 and Table 1). especially that for dry deposition. 4a).7 kg N ha-1 yr-1) from fires in Indonesia and Peninsular Malaysia. However.. 4b).8 kg N ha-1 yr-1 (Fig. a substantial amount of fire-emitted Nr was transported equatorward and 15 . 2). Evergreen broadleaf forests were distributed mostly between 5°N and 5°S and were bordered to the north and south by savannas (Fig. The southern part of South China Sea also received substantial N deposition (up to 2. A small amount of the N from African fire emissions was transported across the Atlantic and deposited over South America. Redistribution of N between ecosystems in Africa Fires caused a net transport of N from savannas to interior forests in tropical Africa (Fig. BNF was highest near the equator and decreased to the north and south with decreasing ET (Fig. received high N deposition fluxes – up to 3. owing to high levels of fire emissions in Africa and the prevalent westerly wind during the fire season (see Fig.

Convective lifting of air masses near the equator increased precipitation and. received relatively small N deposition fluxes from fire emissions. respectively. which were located upwind of the African savanna regions during the fire seasons in the northern and southern hemispheres. 4c). when winds to the north carried emissions from SH savannas to interior tropical forests.deposited in tropical forests. which corresponded to the NH fire season. atmospheric transport. The combined effects of biomass burning emissions. wet deposition. Prevailing winds in South America and Southeast Asia also caused transport of fire emissions toward interior (and relatively undisturbed) areas of the Amazon and the Indonesian archipelago (Fig. 4f and Fig. subsequently. In NH winter. 16 . prevailing winds were to the south (Fig. The Sahara and Kalahari deserts. S4). 2c). and deposition resulted in a net transport of N from savannas to forests in Africa (Fig. The transport was reversed in NH summer. This equatorward transport pattern was not unique to Africa.

2008). 2004) of long-term increases in carbon storage observed within Amazonian (Phillips et al. 2009) forests..g.DISCUSSION AND CONCLUSIONS We estimated emissions and deposition of N from tropical fires. we found an equatorward transport of N from fires in savannas and at active deforestation frontiers to interior. Most fires occurred in savannas and in areas that were undergoing active deforestation. Our results indicated a redistribution of N between different types of tropical ecosystems. Although modeling studies suggest tropical forests have great potential to increase net primary production in response to elevated levels of carbon dioxide (Friedlingstein et al.. toward the Intertropical Convergence Zone (ITCZ) (See Fig. 2006. the net transport of N from savannas to forests in Africa was larger than that observed in South America or Asia. A significant amount of N from this zonal transport was removed by wet and dry deposition over relatively undisturbed tropical forests. Specifically. As a consequence of widespread savanna burning in Africa. the prevailing winds carried fire emissions from savannas to tropical forest during both NH and SH fire seasons. Interior tropical forests gained N equivalent to 4% of their BNF.. This atmospheric transport of N was closely related to the seasonality of fire emissions and meteorological patterns in tropics.. a key uncertainty is whether nutrient availability can keep pace with photosynthesis to allow for long-term increases in 17 . S4). Lewis et al.. In tropical Africa.. Ciais et al. The Hadley circulation carried emissions from these fires equatorward. The cross biome transport of N described here strengthens the case for increases in nutrient deposition serving as a key driver (e. intact tropical forests. fire N losses were equivalent to 28% of BNF in savannas and 38% of BNF for ecosystems at the deforestation frontier. 2009) and African (Lewis et al. On average.

2007). free air carbon dioxide enrichment studies from mid-latitude forests show that rates of carbon accumulation in response to elevated levels of carbon dioxide increase when nutrient availability is enhanced (Oren et al. and land use in neighboring savanna regions may be enhancing nutrient availability in nearby tropical forest ecosystems– and thus increasing the sensitivity of these ecosystems to changing levels of atmospheric CO2.biomass (e. Luo et al.. Satellite-based fire detections suggest that fire use for pasture and cropland management sustains high fire activity following deforestation (Schroeder et al. 2005). Indeed. The impacts of these deposition fluxes for carbon accumulation may be largest in younger secondary forests where nitrogen and phosphorous limitation are most pronounced (Davidson et al.. management of deforested areas.g.. 2001). may additionally increase the nutrient loading to forests near the deforestation frontier. In parallel to the patterns shown here for N.. Other land use-related changes in nutrient cycling.. increased nutrient loading by deposition of fire emissions in intact and secondary tropical forest ecosystems may partially offset some of the carbon losses associated with tropical deforestation. 2004. fire-emitted black carbon aerosols have been shown to contribute in important ways to phosphorous deposition in tropical forests within the Amazon (Mahowald et al. 2003. 2004).. it is 18 . including the use of N fertilizer in agriculture after forest clearing and increases in dust. the net effect of the advancing deforestation frontier is therefore to expand the area under fire management and to increase the proximity of savanna fires to highly productive interior forests. In terms of assessing the net impact of land use change on global levels of atmospheric CO2. In this context.. Our analysis shows how concentrated fire use for deforestation. Davidson et al.. Hungate et al. 2005).

Further work is needed to identify how nutrient loading from fires affects marine ecosystem function in these highly impacted areas. A large portion (~37%) of N from savanna and forest fires is carried to and deposited over tropical oceans (Table 1). this deposition is relatively small (2%) compared to BNF and also with respect to N transport to surface waters by upwelling (Capone et al. decomposition and fire carbon loss pathways from deforestation may not lead to substantially different outcomes. In terms of atmospheric CO2 levels. currently there are not enough observations to derive a global map of ocean N fixation (Capone et al. 2007). First... Averaged over the whole tropical ocean. ozone. However.g. 2003). changes in aerosol optical depth and diffuse light (Oliveira et al. However. In equatorial Asia after the 1997/1998 El Nino. 2005).. Doughty et al. N is generally considered a primary limiting nutrient for phytoplankton biomass accumulation in marine ecosystems. particularly in coastal systems (Rabalais. and human health impacts. 2005). including phytoplankton primary production and the health of coral reefs.important to further refine our understanding of the fire-emitted component of deforestation carbon losses (e. DeFries et al. 2009. 2009). increases in atmospheric N deposition by anthropogenic activity may be partially offset by lower rates of N fixation (Krishnamurthy et al. these loss pathways are fundamentally different. Nevertheless.. 19 .. for redistribution of nutrients. 2007. Detailed analysis of the effect of atmospheric N deposition on marine ecosystems is complex for several reasons. Second.. 2002).. Mercado et al.. methane. coral reef death was attributed to extraordinary red tide caused by deposition of iron from fire emissions (Abram et al.. for example. 2008). the ratio is much higher in coastal regions in Africa and Southeast Asia (Table 1).

gov/DEBITS. http://www. Better measurements are required to improve the model simulation of N transport and deposition. an improved understanding of the fate of N lost during deforestation and N cycling during post-deforestation land use may enable us to better quantify human impacts on N cycling in tropical ecosystems. More detailed measurements of N losses to N2 during fires also are needed to reduce uncertainties associated with pyrodenitrification. the Deposition of Biogeochemically Important Trace Species (DEBITS) network. 20 . A quantitative understanding of this transport pathway is currently limited by several different types of observations.igac.g..php). Although considerable effort has gone into improving our understanding of the deposition of chemical species in tropics (e.Here we show that N emissions from savanna and deforestation fires lead to deposition in tropical forest ecosystems as a consequence of atmospheric transport associated with the ITCZ. including N deposition measurements near deforestation regions and improved estimates of fire emissions associated with deforestation. Finally. measurements of tropical N deposition are still sparse compared to the density of available observations in temperate regions.noaa.

The GEOS-Chem model is managed by the Atmospheric Chemistry Modeling group at Harvard University with support from the NASA Atmospheric Chemistry Modeling and Analysis Program. 21 . Kasibhatla P.S.ACKNOWLEDGEMENTS This work was funded by NASA NNX08AF64G. was partially supported by the grant NNX08AL03G from Duke University.

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31 1.83 0.51 0.22 4.62 0.69 9.04 0.70 0.Table 1. 2 3 Estimated using the mean of central and conservative regressions between BNF and ET as given in Cleveland et al.80 0.15 1. ‘Total tropics’ refers to regions within 30°S-30°N. 2.32 -7.01 4.94 2..88 5.22 0. South America.17 0.34 0 0.46 -0.16 0.75 2.87 2.67 0. (1999).39 0.01 10.34 1.04 0.55 3.42 2.59 0.01 4.12 0.29 15.56 -1. N fluxes from fires over tropical regions1.21 0. and Southeast Asia are shown in Fig.83 20.46 13. 31 .12 0.32 0 2. In this study. Here it is defined as region with forest cover greater than 10% and the fraction of forest loss during 2000-2005 (Hansen et al.05 0.82 -0.21 0.12 0.85 % of BNF -3 16 -5 -39 6 -4 1 -21 -10 3 -35 8 -60 -35 6 -10 4 -38 -28 2 288 123 5 921 2966 693 390 64 397 1494 304 16 56 112 2523 1409 529 145 1610 19530 Frontier4 Savanna Ocean Tropical forest Interior South America Frontier Savanna Ocean Tropical forest Interior Southeast Asia Frontier Savanna Ocean Tropical forest Interior Total tropics Frontier Savanna Ocean 1 The domains of tropical regions in Africa.36 1.01 0.11 Fire emissions of Nr Tg N yr-1 0. 4 ‘Frontier’ refers to tropical forest region undergoing substantial anthropogenic deforestation.13 0.64 0.63 0. The values are 10 year (1997-2006) averaged.54 0.66 120. ‘Interior’ refers to tropical forest region that is rarely affected by human activities.5° grid cell with fraction of evergreen broad leaf forest (from MODIS 500 m land cover product) over 70% and the 10-year average fire emission rate (from GFEDv2) smaller than 500 kg C ha-1 yr-1.87 -2.01 0.44 27. Area Continent Region Mha Tropical forest Interior Africa 3 Biological Nitrogen Fixation2 Tg N yr-1 5.19 0.03 -0.19 1.80 28.07 -0.07 0.28 -1.54 0.07 0. 2008) greater than 1%.31 -0.70 2.24 0.21 -0.52 12.51 8.85 % of BNF 20 19 13 14 6 4 2 8 5 3 13 13 18 9 6 9 6 12 10 2 Net fire N flux Tg N yr-1 -0.67 0.86 5.01 2.04 0.03 0 Fire emissions of N2 Tg N yr-1 0.81 0.28 0.21 0.00 0 0.01 -6.66 0.49 0.32 0 2.90 0.52 0.63 0 1.70 0.11 15.41 0 Deposition of fireemitted N Tg N yr-1 1.61 0.69 0.58 0 1. it is defined as 2°×2.

FIGURE CAPTIONS Figure 1: Comparison of observed and modeled N wet and dry deposition rates (kg N ha-1 yr-1) in tropical regions. The values are in kg N ha-1 yr-1. South America. (e) N deposition from biomass burning. and in Southeast Asia. Solid pink boxes define the domains of tropical Africa (AFR). Red and blue points represent deposition rates for oxidized N (NO3-N) and reduced N (NH4-N). Blue and red colors represent N addition to and loss from terrestrial ecosystems. respectively. with northward wind denoted as positive. Figure 4: Latitudinal distributions of mean (a) fraction of forest and savanna cover. circles. The values are the 10 year (1997-2006) mean from the GEOS-Chem simulation. 1:2. (1999) using a global map of ET from Fisher et al. (c) meridional wind speed (m/s) at 850hPa. Gray points are observation stations near urban areas. Dashed lines indicate 1:1. and 2:1 relationships. (b) N deposition from biomass burning. South America. Filled diamonds. and triangles represent data for Africa. (b) biological N fixation (kg N ha-1 yr-1) estimated from Cleveland et al. Red and blue solid lines show linear regression fits for NO3-N and NH4-N deposition rates. (d) N emissions from fires. respectively. tropical South America (SAM). The net fire N flux includes both losses from Nr and N2 emissions and gains from N deposition. and (f) net fire N and Nr fluxes (kg 32 . Figure 3: Seasonal variability of total dry and wet deposition (Tg N yr-1) of N from biomass burning over NH Africa. (2008). and (c) net fire N flux with respect to the surface. SH Africa. Figure 2: Simulated 10-year average (a) N emissions from fires (the sum of Nr and N2). and tropical Southeast Asia (SEA) used in this paper. and Southeast Asia (the domains are defined in Fig. 2).

the Sahara desert. from north to south. derived from GEOS-4 reanalysis data. 10°E-30°E). and the Karahari desert in Southwest Africa. The net fire Nr flux includes losses from Nr emissions and gains from N deposition. tropical forest. The values are 10 year (1997-2006) averaged. This domain covers. The meridional wind speed. is averaged over February (representing fire season in NH) and August (representing fire season in NH).N ha-1 yr-1) for tropical African region (30°S-30°N. NH savanna. SH savanna. 33 .

Figure 1 34 .

Figure 2 35 .

Figure 3 36 .

Figure 4 37 .

CO/CO2 ratio Figure S2 Forest cover loss due to deforestation and tropical ecosystem masks Figure S3 Biomass emission and wind vectors Table S1 Summary of N deposition observations Table S2 N fluxes from fires in tropical regions– expressed in units per unit of land area 38 .SUPPORTING INFORMATION The following Supporting Information is available for this article: Figure S1 N2-N/Nr-N ratio vs.

The dash-dotted. 39 .Figure S1. tropical forest fires.. dashed. respectively. 1991). We also excluded three wood points below the N2 detection limit. Data are based on results from a chamber experiment (Kuhlbusch et al. excluding two pine needles samples (gray points) because of the limited abundance of conifer plant functional types in tropical regions. N2-N/Nr-N ratio as a function of CO/CO2 ratio. and extratropical forest fires. and dotted vertical lines represent the CO/CO2 values for savanna fires.

(2008).5º resolution. The original data were compiled by Hansen et al.Figure S2. (d) Tropical ecosystem masks in 2º×2.5º×0.5º cell. The tropical ecosystem cover fractions and masks were derived from MODIS 500 m land cover product. (a) Deforestation within the humid tropics during 2000-2005. shown as the percent loss within each 0. (c) Tropical savanna cover fraction (%). (b) Tropical forest cover fraction (%). 40 .

2.Figure S3. The values are 10 year (1997-2006) averaged. 41 . Latitudinal distribution of Nr emission and deposition rates (kg N ha-1 yr-1) from fire and other sources. Inserted plots show the mean values and fire contribution fractions for three tropical regions as defined in Fig.

2004. 42 . Red shaded areas depict the Nr emissions (kg N ha-1 yr-1) from biomass burning for these months (10-year average).Figure S4. The full length of an arrow represents a wind speed of ~20m/s. The GEOS-4 wind vectors at 850hPa in tropical regions for February and August.

2002 05/1998-04/2003 04/1999-02/2001 1999 08/1997-07/1998 Aug-Mar. RSA Africa Lamto.. Niger Louis Trichardt.99 1.28 0. 2003 Galy-Lacaux et al.. 2007. 2008 Boy et al.78 0.52 0..02 (EANET).97 (kg N ha-1 yr-1) 3.02 2. 2009 Galy-Lacaux et al.60 1.cc EANET 3º10' N 13º20' N 23º00' S 6º N 25º S 13º20' N 12º30' N 10º04' S 4º S 21º48' S 5º21' S 22º54' S 4º S 4º S 10º04' S 10º04' S 10º04' S 4º28' N 11º58' E 2º25' E 30º02' E 5º W 31º38' E 2º25' E 8º5' W 61º56' W 79º05' W 48º11' W 53º41' W 47º03' W 79º05' W 79º05' W 61º56' W 61º56' W 61º56' W 101º22' E 09/1996 – 04/2000 06/1996 – 10/1996 1986 ...97 2.18 1. Brazil Andean montane forest. Ecuador Araraquara.38 (kg N ha-1 yr-1) 4.23 0.58 1. Brazil Rondônia.06 1. Indonesia 0º12' S 100º19' E 2000 – 2005 4. Ecuador Andean montane forest.03 0...92 2. RSA Banizoumbou.42 0.. Côte d'Ivoire Skukuza.22 0.07 2. 2008 Trebs et al.62 2.2005 8. 2002 Acid deposition Monitoring Network in East Asia NO3-N (mod) NH4-N (obs) NH4-N (mod) Reference 43 .00 0. 2008 Da Rocha et al.08 1.73 4.10 0. 2005 Yoboué et al..1999 1995 .. Averaged over 4 sites Boy et al. 2006.88 0. Niger Katibougou. 2009 Yoboué et al.29 0.60 0. Brazil Rondônia. Brazil Andean montane forest. 2009 Trebs et al..10 0.. 1998-2003 Apr-Jul.90 0.07 3..57 4. Cameroon Banizoumbou. Indonesia Asia Kototabang.73 1..00 1.56 2. value in kg N ha -1 month-1 Trebs et al.eanet.56 0.26 1.81 0.80 0.80 1.14 6º15' S 106º34' E 2001 . Mali Rondônia. The shaded rows represent dry deposition measurements and other rows represent wet deposition measurements.13 0..67 1.88 1.44 2. 2005 Lara et al.93 0.83 1.95 2. 2005 Mphepya et al.63 0.60 0.53 1... 1998 Mphepya et al. value in kg N ha -1 month-1 Ayers et al. Brazil Petit Sault. Data available online: http://www.09 0.2002 07/1999-06/2002 06/1994-09/2005 1997-2005 Sep-Nov. 2006 Galy-Lacaux et al.26 1.28 0.71 0. value in kg N ha -1 month-1 Trebs et al.89 1. List of wet and dry N deposition observations and corresponding simulated values at non-urban sites in tropical regions.25 0.84 1. 2006 Boy et al.06 2.Table S1.26 11. Updated in Galy-Lacaux et al. NO3-N (obs) Region Location Latitude Longitude Time (kg N ha-1 yr-1) Zoétélé. 1998-2003 09/2002 10/2002 11/2002 1996 1. 2006.96 (kg N ha-1 yr-1) 1.83 Sigha-nkamdjou et al. 2004. 2006.20 0.75 0..84 0.52 0.63 1.57 0.29 2.05 2.83 2. Ecuador Rondônia.04 0..20 0. Malaysia Southeast Serpong.86 0.67 0. French Guyana South America Piracicaba River Basin.09 0. Brazil Tanah Rata.08 2.83 1.24 0.31 0.86 0.

53 2.69 EANET EANET EANET EANET EANET EANET 44 .08 3.62 0.74 10.93 3.16 1.95 6.2005 2.31 2. Malaysia Patumthani.66 1.01 2.Tanah Rata.93 5.31 1.55 1. Thailand Vachiralongkorn Dam. Thailand Mae Hia.23 1.48 3.07 1.08 3. Thailand Khao Lam.55 2. Vietnam 4º28' N 14º02' N 14º4' N 14º46' N 18º46' N 20º49' N 101º22' E 100º46' E 101º37' E 98º35' E 98º56' E 105º20' E 2000 – 2005 2000 – 2005 2000 – 2001 2002 – 2005 2001 – 2005 2000 .71 1.01 5.59 2. Thailand Hoa Binh.58 4.93 0.

3 0.2 1.4 -1.7 0.2 6.7 -1.2 -6.1 % of BNF 20 19 13 14 6 4 2 8 5 3 13 13 18 9 6 9 6 12 10 2 Net fire N flux kg N ha-1 yr-1 -0.4 25.3 -2.4 30.1 -9.3 1.6 0 3.9 3.4 0.5 25.4 0.8 25.0 1.2 5.1 0 Fire emissions of N2 kg N ha-1 yr-1 2.4 3.6 3.1 % of BNF -3 16 -5 -39 6 -4 1 -21 -10 3 -35 8 -60 -35 6 -10 4 -38 -28 2 45 .2 3.4 25.4 30.5 0.2 6.5 1.0 0.3 1.4 0.8 25.9 0.0 0.4 25.4 30.9 1.8 -14.7 0 1.7 4.4 9.9 0.9 2.1 -4.3 1.8 0.2 4.8 0 1.1 4.2 6.5 2.Table S2.5 -4.4 25.9 0.2 Fire emissions of Nr kg N ha-1 yr-1 2.2 -5.4 25.5 9.2 1.5 0 3. Same as Table 1 but expressed in units per unit of ecosystem area (kg N ha-1 yr-1).5 2.3 2.0 0. Area Continent Region Mha Tropical forest Interior Africa Frontier Savanna Ocean Tropical forest Interior South America Frontier Savanna Ocean Tropical forest Interior Southeast Asia Frontier Savanna Ocean Tropical forest Interior Total tropics Frontier Savanna Ocean 288 123 5 921 2966 693 390 64 397 1494 304 16 56 112 2523 1409 529 145 1610 19530 Biological Nitrogen Fixation kg N ha-1 yr-1 25.4 0 Deposition of fireemitted N kg N ha-1 yr-1 4.3 2.9 1.8 0.7 0.1 4.1 0.4 25.4 25.1 3.2 5.9 0.9 -2.2 3.2 -4.2 2.8 0 1.0 0.4 25.3 0 0.2 6.8 1.0 2.3 0.5 1.4 30.

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