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

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.

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.,

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

N deposition across both terrestrial and ocean ecosystems. Emissions of NO and NH3 probably account for only 40-50% of the N present in fuels prior to combustion, as some is retained within the ecosystem in combusted residues (approximately 20%) and the remainder (another 3040%) is transformed directly into N2 during the combustion processes (Lobert et al., 1990; Kuhlbusch et al., 1991). 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, we assessed the contribution of fires to N cycling in tropical ecosystems. We explored the loss of N by emissions from biomass burning and the gain of Nr by deposition from the atmosphere. We estimated fire emissions using the Global Fire Emission Database version 2 (GFEDv2, van der Werf et al., 2006), which combines satellite observations of burned area (Giglio et al., 2006) and a biogeochemical model constrained by other satellite data to estimate fuel loads. We estimated N2 emissions from biomass burning using data derived from a chamber burning experiment (Kuhlbusch et al., 1991). The transport and deposition of N were simulated by using the GEOS-Chem global chemical transport model (CTM) (Bey et al., 2001). We performed 10 years (19972006) of global-scale simulations but focus our analysis and discussion on tropical ecosystems. We validated some of our modeled fluxes by comparing our results with published observations of N deposition. We also estimated the net N flux from fire emissions in different tropical ecosystems. These fluxes were then compared with terrestrial and marine BNF fluxes (Cleveland et al., 1999; Deutsch et al., 2001; Lee et al., 2002).

METHODS
Nr emissions from biomass burning The GFEDv2 product consists of 11 gridded monthly burned area (BA), fuel loads (FL), combustion completeness (CC), and emissions factors (EMFs) for different gas and aerosol species (van der Werf et al., 2006). Burned area was derived using Moderate Resolution Imaging Spectroradiometer (MODIS) active fire and burned area datasets as described by Giglio et al. (2006). 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., 2003, 2006). 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. Emission factors, defined as the emission of species (g) per 1 kg burned DM, were obtained from Andreae and Merlet (2001). Comparison with atmospheric carbon monoxide (CO) observations provides some validation of carbon emissions. GFEDv2 CO emissions in equatorial Asia, for example, 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., 2008). CO anomalies from GFEDv2 in the GEOS-CHEM model had a mean correlation of 0.79 with observations from NOAA Global Monitoring Division (GMD) stations in the Northern Hemisphere

and 0.59 with GMD stations in the Southern Hemisphere (Kai et al., 2009). Similarly, the ratio of modeled to observed standard deviations of CO anomalies from GMD was 0.86 and 1.09, respectively, for northern and southern hemispheres. These results indicate that while emissions estimates are still uncertain, they are of sufficient quality to study the impact of fire-emitted species on atmospheric composition. Nr can be emitted into the atmosphere in different chemical forms and physical phases. NOx and NH3 account for the majority (greater than 90%) of Nr emissions from biomass burning (Andreae and Merlet, 2001). In our model simulations and calculations, we used the sum of gaseous NOx and NH3 emissions to represent total Nr emissions from biomass burning. The low bias we expect from neglecting the remaining Nr emissions (e.g., N2O, HCN, and acetonitrile) is small compared with uncertainties associated with our estimates of burned area (e.g., Giglio et al., 2006) and total carbon emissions (e.g., van der Werf et al., 2008).

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., 1990). By burning different biomass materials in a stainless steel chamber, Kuhlbusch et al. (1991) showed that the missing N is mostly molecular N (N2), which accounts for approximately one third of fuel N. 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. CO/CO2 emission ratio

serves as a powerful indicator for the relative extent of flaming combustion and smoldering combustion. Analysis of the Kuhlbusch et al. (1991) measurements showed that the N2-N to Nr-N ratio of fire emissions was inversely related to its CO/CO2 ratio (see Fig. S1 in Supporting Information). The N2-N to Nr-N ratio derived from this relationship was used to estimate global N2 emissions from biomass burning. In this study, we estimated the CO/CO2 ratio for three different fire types: savanna and grassland fires, tropical forest fires, and extratropical forest fires using the emission factors of CO and CO2 listed in Table 1 of Andreae and Merlet (2001). A 2(latitude) 2.5(longitude) vegetation map of these three types (Andreae and Merlet, 2001) was used to derive the global gridded N2-N to Nr-N ratio. For each grid cell, the GFEDv2 Nr emission rate was scaled by this ratio to approximate the fire emission rate of N2.

Model simulations of N transport and deposition We used the GEOS-Chem model to calculate the transport, transformation, and deposition of biomass burning emitted N species. GEOS-Chem is a global 3-D CTM (Bey et al., 2001) driven by assimilated meteorological observations from the Goddard Earth Observing System (GEOS) of the NASA Global Modeling and Assimilation Office (GMAO). In this study, we used version 08-01-01 of the model with 22.5 horizontal resolution and 30 vertical layers between the surface and 0.01 hPa. The GEOS-Chem model includes a detailed description of tropospheric O3-NOx-hydrocarbon chemistry (Wang et al., 1998). Emission sources of N include NOx from lightning, soil and fertilizer, aircraft, biofuel, fossil fuel, biomass burning, and NH3 from biofuel, fossil fuel, biomass burning, and

natural sources (e.g., soils, vegetation, and wild animals). N tracers are present in gas phase (e.g., NOx, peroxyacyl nitrate (PAN), HNO3, N2O5, and NH3) or aerosol phase (NH4+, N on sulfate, and N on sea salt). These tracers are transported by meteorology-driven advection and convection processes, and finally removed by the action of precipitation (wet deposition) or by contact with surface or vegetation (dry deposition). We performed GEOS-Chem full chemistry simulations over a 10-year period (1997-2006) using the GFEDv2 inventory, which resolves the interannual variability of biomass burning emissions. N emissions from other sources were obtained from climatological inventories which represent contemporary (circa 2000) emissions. After a three-month spin-up period with the same initial conditions, two sets of simulations were conducted: one with biomass burning emissions prescribed from GFEDv2, and another without these emissions. The difference between these two simulations represents the effect of biomass burning emissions on N transport and deposition. We recorded monthly mean deposition rates for each N species through dry and wet deposition. Wet deposition included convective and large-scale components (Liu et al., 2001). Total deposition rate of N from biomass burning was then calculated for each 22.5 model grid cell.

Biological N fixation Cleveland et al. (1999) reviewed published studies and generated three linear regressions (conservative, central, and upper-bound) between BNF and evapotranspiration (ET) in terrestrial ecosystems. Galloway et al. (2004) argued that the true N fixation rate lies at the lower end of this

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

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RESULTS
Validation of wet and dry deposition Relative to Northern Hemisphere industrial regions, fewer N deposition measurements exist for tropical land and ocean regions. Here we compiled wet and dry N deposition measurements in tropical regions published in recent years. We only considered observations from 1996 to 2006 to ensure overlap with the period of our satellite-derived fire emissions time series. 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. Based on the original data, 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. Altogether, we reported wet and dry deposition rates from 26 non-urban stations. The location and time period of these measurements, as well observed and modeled deposition rates, are summarized in Table S1. We compared these observations with modeled deposition fluxes, which were sampled in grid cells corresponding to observations during the month when observations were available. For locations that had measurements only during 1996, we compared the deposition rates with our 10-year (19972006) mean model results. Overall, the model simulation corresponded reasonably well to wet and dry deposition observations at non-urban sites (Fig. 1). About 75% of the wet deposition rates and 80% of the dry deposition rates agreed within 50% with the observations. This agreement was similar to previous comparisons of N deposition between models and observations (Lamarque et al., 2005; Dentener et al., 2006). The model somewhat underestimated NO3-N wet deposition and overestimated NH4-N dry deposition.

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Simulations were more strongly correlated with measurements for dry deposition than for wet deposition, as indicated by the r values shown in Fig. 1. In contrast to non-urban sites, the model was generally biased low relative to the high urban data, which were likely affected by nearby fossil fuel emissions (Fig. 1). Urban data were generally not representative of the 22.5 grid cells in the model, so they were not included in our linear regressions. We note most of these urban measurement sites were located in Southeast Asia.

Gross N emissions from fires Emissions of Nr and N2 by fires were 10.4 Tg N yr-1 (6.5 kg N ha-1 yr-1) in savannas and 5.3 Tg N yr-1 (3.8 kg N ha-1 yr-1) in tropical forests, with these two biomes accounting for 67% of global fire N emissions (Fig. 2a and Table 1). High emission rates occurred in African savannas, as well as in deforestation regions (See Fig. S2) in South America and Southeast Asia. Losses directly to N2 accounted for about half of the total N emissions flux. 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. S3). Deposition rates were highest near source regions - with maxima on the perimeter of the Congo basin in Africa (up to 9.9 kg N ha-1 yr-1), in southern Borneo in equatorial Asia (up to 9.7 kg N ha-1 yr-1), and across the Brazilian state of Mato Grosso, eastern Bolivia, and Paraguay in South America (up to 5.3

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kg N ha-1 yr-1) (Fig. 2b). These results imply that undisturbed forest and savanna ecosystems in these regions (e.g. parks and other protected areas) experience relatively high N deposition from nearby deforestation and savanna fires. Seasonal variations in N deposition were closely linked with the timing of fire emissions (Fig. 3). Total wet deposition was comparable to total dry deposition across the tropics, although regionally the relative importance of these two pathways varied. 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%). About 2/3 of the total N wet deposition occurred in the gas phase (NH3 and HNO3). The relative importance of wet deposition as an atmospheric loss pathway increased towards the end of the fire season on all three continents (Fig. 3), probably as a consequence of increasing precipitation levels. Model estimates of the total deposition rate for oxidized N and reduced N were similar. Separation of N deposition by its oxidation form is important for assessing N deposition effects on ecosystem function. Reduced N, for example, can reduce base cation uptake by plants (de Graaf et al., 1998), causing changes in species composition in ecosystems such as heathlands (van der Berg et al., 2008) and peatlands (Paulissen et al., 2004).

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. Savanna ecosystems in Africa and South America and tropical deforestation frontiers in all three regions experienced a net loss of N (Figs. 2c, S2). Net gains at a

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regional scale occurred in interior tropical forests and over tropical oceans. The net loss of N (Nr and N2) from savanna ecosystems was largest in Africa (Table 1), where fire return times were lower than on other continents (Giglio et al., 2006; Van der Werf et al., 2008). Net fire losses were equal to approximately 39% of BNF in savanna ecosystems in Africa, corresponding to 6.19 Tg N yr-1 or 6.7 kg N ha-1 yr-1 in savanna ecosystems (Table S2). Of the directly emitted Nr from African savanna fires, only 53% was returned to savannas via deposition. Most of the remainder was deposited in downwind tropical forests (e.g., in the Congo basin) and over the tropical Atlantic Ocean (Fig. 2b). For savannas across all three continents, net fire N losses were equal to 28% of BNF (4.8 kg N ha-1 yr-1), with 55% of Nr emissions remaining within these ecosystems via deposition in nearby areas. Tropical forests received large N deposition inputs from savanna fires but also lost N through deforestation fires. Overall, tropical forest fires had a net N loss equal to approximately 10% of BNF (2.83 Tg N yr-1 or 2.0 kg N ha-1 yr-1). In Southeast Asia, net losses were higher (35%), because a larger proportion of fire emissions were associated with deforestation in tropical forests. 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), the net effect of remote tropical fires was an increase atmospheric deposition. For interior forests in Africa, for example, the net atmospheric flux from fires was 0.46 Tg N yr-1 (3.7 kg N ha-1 yr-1), corresponding to approximately 16% of BNF. In contrast, forests at the deforestation frontier in South America and Southeast Asia had a large net N loss at a regional scale from fire emissions. Expressed as a percentage of BNF, net N losses at the deforestation frontier (38%) were

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even higher than in savanna ecosystems. Tropical oceans were a large recipient of N from fire emissions. Approximately 37% (2.85 Tg N yr-1) of fire-emitted N was deposited over oceans. The tropical Atlantic, in particular, received high N deposition fluxes up to 3.8 kg N ha-1 yr-1 (Fig. 2), owing to high levels of fire emissions in Africa and the prevalent westerly wind during the fire season (see Fig. S4). A small amount of the N from African fire emissions was transported across the Atlantic and deposited over South America. 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., 2009). The southern part of South China Sea also received substantial N deposition (up to 2.7 kg N ha-1 yr-1) from fires in Indonesia and Peninsular Malaysia.

Redistribution of N between ecosystems in Africa Fires caused a net transport of N from savannas to interior forests in tropical Africa (Fig. 2 and Table 1). Evergreen broadleaf forests were distributed mostly between 5N and 5S and were bordered to the north and south by savannas (Fig. 4a). BNF was highest near the equator and decreased to the north and south with decreasing ET (Fig. 4b). The highest levels of Nr and N2 fire emissions occurred at ~7N in the northern hemisphere and ~10S in the southern hemisphere. The N deposition pattern, especially that for dry deposition, was similar to that of fire emissions but with a small equatorward shift in peak deposition in the NH. A portion of Nr emitted from savanna fires was deposited back in savannas. However, a substantial amount of fire-emitted Nr was transported equatorward and

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

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DISCUSSION AND CONCLUSIONS

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

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biomass (e.g., Hungate et al., 2003; Luo et al., 2004). Indeed, 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., 2001). Our analysis shows how concentrated fire use for deforestation, management of deforested areas, 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. Satellite-based fire detections suggest that fire use for pasture and cropland management sustains high fire activity following deforestation (Schroeder et al., 2005); 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 parallel to the patterns shown here for N, 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., 2005). Other land use-related changes in nutrient cycling, including the use of N fertilizer in agriculture after forest clearing and increases in dust, may additionally increase the nutrient loading to forests near the deforestation frontier. 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., 2004, Davidson et al., 2007). In terms of assessing the net impact of land use change on global levels of atmospheric CO2, 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. In this context, it is

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

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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. A quantitative understanding of this transport pathway is currently limited by several different types of observations, including N deposition measurements near deforestation regions and improved estimates of fire emissions associated with deforestation. More detailed measurements of N losses to N2 during fires also are needed to reduce uncertainties associated with pyrodenitrification. Although considerable effort has gone into improving our understanding of the deposition of chemical species in tropics (e.g., the Deposition of Biogeochemically Important Trace Species (DEBITS) network,

http://www.igac.noaa.gov/DEBITS.php), measurements of tropical N deposition are still sparse compared to the density of available observations in temperate regions. Better measurements are required to improve the model simulation of N transport and deposition. Finally, 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.

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ACKNOWLEDGEMENTS
This work was funded by NASA NNX08AF64G. Kasibhatla P.S. was partially supported by the grant NNX08AL03G from Duke University. 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.

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Table 1. N fluxes from fires over tropical regions1. The values are 10 year (1997-2006) averaged.

Area Continent Region Mha Tropical forest Interior Africa

3

Biological Nitrogen Fixation2 Tg N yr-1 5.94 2.90 0.11 15.83 20.29 15.69 9.31 1.51 8.01 10.22 4.67 0.34 1.36 1.46 13.80 28.52 12.55 3.44 27.66 120.11

Fire emissions of Nr Tg N yr-1 0.67 0.04 0.01 4.00 0 0.64 0.07 0.21 0.58 0 1.16 0.01 0.52 0.32 0 2.70 0.12 0.86 5.03 0

Fire emissions of N2 Tg N yr-1 0.69 0.04 0.01 4.34 0 0.66 0.07 0.22 0.63 0 1.05 0.01 0.54 0.32 0 2.62 0.12 0.88 5.41 0

Deposition of fireemitted N Tg N yr-1 1.19 0.54 0.01 2.15 1.21 0.61 0.21 0.12 0.39 0.28 0.59 0.04 0.24 0.13 0.87 2.49 0.80 0.42 2.75 2.85 % 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 -0.17 0.46 -0.01 -6.19 1.21 -0.70 0.07 -0.31 -0.81 0.28 -1.63 0.03 -0.82 -0.51 0.87 -2.83 0.56 -1.32 -7.70 2.85 % 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

The domains of tropical regions in Africa, South America, and Southeast Asia are shown in Fig. 2. Total tropics refers to regions within 30S-30N.

2 3

Estimated using the mean of central and conservative regressions between BNF and ET as given in Cleveland et al. (1999). Interior refers to tropical forest region that is rarely affected by human activities. In this study, it is defined as 22.5 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.

Frontier refers to tropical forest region undergoing substantial anthropogenic deforestation. Here it is defined as region with forest cover greater than 10% and the fraction of forest loss during 2000-2005 (Hansen et al., 2008) greater than 1%.

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

32

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

33

Figure 1

34

Figure 2

35

Figure 3

36

Figure 4

37

SUPPORTING INFORMATION
The following Supporting Information is available for this article: Figure S1 N2-N/Nr-N ratio vs. 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

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

39

Figure S2. (a) Deforestation within the humid tropics during 2000-2005, shown as the percent loss within each 0.50.5 cell. The original data were compiled by Hansen et al. (2008). (b) Tropical forest cover fraction (%). (c) Tropical savanna cover fraction (%). (d) Tropical ecosystem masks in 22.5 resolution. The tropical ecosystem cover fractions and masks were derived from MODIS 500 m land cover product.

40

Figure S3. 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. 2. The values are 10 year (1997-2006) averaged.

41

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

42

Table S1. List of wet and dry N deposition observations and corresponding simulated values at non-urban sites in tropical regions. The shaded rows represent dry deposition measurements and other rows represent wet deposition measurements.
NO3-N (obs) Region Location Latitude Longitude Time (kg N ha-1 yr-1) Zotl, Cameroon Banizoumbou, Niger Louis Trichardt, RSA Africa Lamto, Cte d'Ivoire Skukuza, RSA Banizoumbou, Niger Katibougou, Mali Rondnia, Brazil Andean montane forest, Ecuador Araraquara, Brazil Petit Sault, French Guyana South America Piracicaba River Basin, Brazil Andean montane forest, Ecuador Andean montane forest, Ecuador Rondnia, Brazil Rondnia, Brazil Rondnia, Brazil Tanah Rata, Malaysia Southeast Serpong, Indonesia Asia Kototabang, Indonesia 012' S 10019' E 2000 2005 4.56 2.00 1.57 4.14 615' S 10634' E 2001 - 2005 8.99 1.26 11.73 4.02 (EANET), Data available online: http://www.eanet.cc EANET 310' N 1320' N 2300' S 6 N 25 S 1320' N 1230' N 1004' S 4 S 2148' S 521' S 2254' S 4 S 4 S 1004' S 1004' S 1004' S 428' N 1158' E 225' E 3002' E 5 W 3138' E 225' E 85' W 6156' W 7905' W 4811' W 5341' W 4703' W 7905' W 7905' W 6156' W 6156' W 6156' W 10122' E 09/1996 04/2000 06/1996 10/1996 1986 - 1999 1995 - 2002 07/1999-06/2002 06/1994-09/2005 1997-2005 Sep-Nov, 2002 05/1998-04/2003 04/1999-02/2001 1999 08/1997-07/1998 Aug-Mar, 1998-2003 Apr-Jul, 1998-2003 09/2002 10/2002 11/2002 1996 1.93 0.84 0.84 1.29 2.56 0.80 1.04 0.60 0.62 2.08 2.44 2.58 1.03 0.23 0.20 0.10 0.06 1.96 (kg N ha-1 yr-1) 1.83 1.25 0.53 1.52 0.60 0.63 0.86 0.29 0.28 0.81 0.63 1.09 0.78 0.67 0.28 0.13 0.08 1.97 (kg N ha-1 yr-1) 3.00 0.88 1.02 2.97 2.83 1.26 1.88 0.67 1.95 2.26 1.92 2.31 0.57 0.42 0.20 0.10 0.05 2.38 (kg N ha-1 yr-1) 4.18 1.71 0.83 2.52 0.80 0.89 1.24 0.60 1.07 2.73 1.07 3.75 0.86 0.90 0.22 0.09 0.06 2.83 Sigha-nkamdjou et al., 2003 Galy-Lacaux et al., 1998 Mphepya et al., 2004. Updated in Galy-Lacaux et al., 2009 Yobou et al., 2005 Mphepya et al., 2006 Galy-Lacaux et al., 2009 Galy-Lacaux et al., 2009 Trebs et al., 2006 Boy et al., 2008 Da Rocha et al., 2005 Yobou et al., 2005 Lara et al., 2007; Averaged over 4 sites Boy et al., 2008 Boy et al., 2008 Trebs et al., 2006, value in kg N ha -1 month-1 Trebs et al., 2006, value in kg N ha -1 month-1 Trebs et al., 2006, value in kg N ha -1 month-1 Ayers et al., 2002 Acid deposition Monitoring Network in East Asia NO3-N (mod) NH4-N (obs) NH4-N (mod) Reference

43

Tanah Rata, Malaysia Patumthani, Thailand Khao Lam, Thailand Vachiralongkorn Dam, Thailand Mae Hia, Thailand Hoa Binh, Vietnam

428' N 1402' N 144' N 1446' N 1846' N 2049' N

10122' E 10046' E 10137' E 9835' E 9856' E 10520' E

2000 2005 2000 2005 2000 2001 2002 2005 2001 2005 2000 - 2005

2.08 3.23 1.07 1.16 1.08 3.71

1.66 1.31 1.62 0.93 0.93 3.01

5.93 5.55 1.59 2.31 2.95 6.55

2.48 3.58 4.53 2.01 2.74 10.69

EANET EANET EANET EANET EANET EANET

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Table S2. Same as Table 1 but expressed in units per unit of ecosystem area (kg N ha-1 yr-1).
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 25.4 25.4 30.2 6.8 25.4 25.4 25.4 30.2 6.8 25.4 25.4 25.4 30.2 5.5 25.4 25.4 25.4 30.2 6.2 Fire emissions of Nr kg N ha-1 yr-1 2.3 0.3 2.1 4.3 0 0.9 0.2 3.3 1.5 0 3.8 0.4 9.2 2.8 0 1.9 0.2 5.9 3.1 0 Fire emissions of N2 kg N ha-1 yr-1 2.4 0.3 2.2 4.7 0 1.0 0.2 3.5 1.6 0 3.4 0.5 9.5 2.8 0 1.9 0.2 6.1 3.4 0 Deposition of fireemitted N kg N ha-1 yr-1 4.1 4.4 3.0 2.3 0.4 0.9 0.5 1.9 1.0 0.2 1.9 2.7 4.2 1.1 0.3 1.8 1.5 2.9 1.7 0.1 % 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 -0.6 3.7 -1.2 -6.7 0.4 -1.0 0.2 -4.9 -2.0 0.2 -5.3 1.8 -14.5 -4.5 0.3 -2.0 1.1 -9.1 -4.8 0.1 % of BNF -3 16 -5 -39 6 -4 1 -21 -10 3 -35 8 -60 -35 6 -10 4 -38 -28 2

45