Soil-Air Mercury Flux near a Large Industrial Emission Source before and after Closure (Flin Flon, Manitoba, Canada).

Prior to its closure, the base-metal smelter in Flin Flon, Manitoba, Canada was one of the North America's largest mercury (Hg) emission sources. Our project objective was to understand the exchange of Hg between the soil and the air before and after the smelter closure. Field and laboratory Hg flux measurements were conducted to identify the controlling variables and used for spatial and temporal scaling. Study results showed that deposition from the smelter resulted in the surrounding soil being enriched in Hg (up to 99 µg g(-1)) as well as other metals. During the period of smelter operation, air concentrations were elevated (30 ± 19 ng m(-3)), and the soil was a net Hg sink (daily flux: -3.8 ng m(-2) h(-1)). Following the smelter closure, air Hg(0) concentrations were reduced, and the soils had large emissions (daily flux: 108 ng m(-2) h(-1)). The annual scaling of soil Hg emissions following the smelter closure indicated that the landscape impacted by smelter deposition emitted or re-emitted almost 100 kg per year. Elevated soil Hg concentrations and emissions are predicted to continue for hundreds of years before background concentrations are re-established. Overall, the results indicate that legacy Hg deposition will continue to cycle in the environment long after point-source reductions.

From the city to the Lake: loadings of PCBs, PBDEs, PAHs and PCMs from Toronto to Lake Ontario.

Loadings from Toronto, Canada to Lake Ontario were quantified and major sources and pathways were identified, with the goal of informing opportunities for loading reductions. The contaminants were polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs), polycyclic aromatic hydrocarbons (PAHs) and polycyclic musks (PCMs). Loadings were calculated from measured concentrations for three major pathways: atmospheric processes, tributary runoff, and wastewater treatment plant (WWTP) effluents. Although atmospheric deposition to the Great Lakes has received the greatest attention, this was the dominant loading pathway for PCBs only (17 ± 5.3 kg/y or 66% of total loadings). PCB loadings reflected elevated urban PCB air concentrations due to, predominantly, primary emissions. These loadings contribute to consumption advisories for nearshore fish. PBDE loadings to the lake, again from mainly primary emissions, were 48% (9.1 ± 1.3 kg/y) and 42% (8.0 ± 5.7 kg/y) via tributaries and WWTPs, respectively, consistent with emissions deposited and subsequently washed-off of urban surfaces and emissions to the sewage system. PAHs loadings of 1600 ± 280 kg/y (71%) from tributaries were strongly associated with vehicle transportation and impervious surfaces. PCM loadings were 83% (±140 kg/y) from WWTP final effluent, reflecting their use in personal care products. Opportunities for source reduction lie in reducing the current inventories of in-use PCBs and PBDE-containing products, reducing vehicle emissions of PAHs and use of PAHs in the transportation network (e.g., pavement sealants), and improving wastewater treatment technology.

Impact of closing Canada's largest point-source of mercury emissions on local atmospheric mercury concentrations.

The Flin Flon, Manitoba copper smelter was Canada's largest point source of mercury emissions until its closure in 2010 after ~80 years of operation. The objective of this study was to understand the variables controlling the local ground-level air mercury concentrations before and after this major point source reduction. Total gaseous mercury (TGM) in air, mercury in precipitation, and other ancillary meteorological and air quality parameters were measured pre- and postsmelter closure, and mercury speciation measurements in air were collected postclosure. The results showed that TGM was significantly elevated during the time period when the smelter operated (4.1 ± 3.7 ng m(-3)), decreased only 20% during the year following its closure, and remained ~2-fold above background levels. Similar trends were observed for mercury concentrations in precipitation. Several lines of evidence indicated that while smelter stack emissions would occasionally mix down to the surface resulting in large spikes in TGM concentrations (up to 61 ng m(-3)), the largest contributor to elevated TGM concentrations before and after smelter closure was from surface-air fluxes from mercury-enriched soils and/or tailings. These findings highlight the ability of legacy mercury, deposited to local landscapes over decades from industrial activities, to significantly affect local air concentrations via emissions/re-emissions.

A comparison of data quality control protocols for atmospheric mercury speciation measurements.

Significant advances in the measurement of atmospheric mercury species have been made in the past 10 years yet limited protocols on quality control (QC) and assurance on this data have been published in the literature. Recently, considerable work has been done to develop quality control and assurance programs within North America. Environment Canada and the National Atmospheric Deposition Network (NADP) independently developed programs, RDMQ™ and AMQC, respectively, to QC atmospheric mercury speciation data (including gaseous elemental mercury (GEM), reactive gaseous mercury (RGM) and mercury associated to particles (PHg)). These 2 programs were assessed by the criteria on which the data is QCed and comparability of the final data products. Results show that the criteria used to flag data compare well within the 4 tested sites and that the number of flags for each criterion is generally comparable. The QC programs were applied to 2 distinct data sets and the final QCed data was compared. From a mid-latitude site, the final data sets compare very well and showed there to be a 0.3, 8.6 and 15% difference in the mean GEM, RGM and PHg concentrations post QC of each program. It is recommended that either the RDMQ or the AMQC programs be employed for a typical mid-latitude site. When the QC programs were applied to highly variable data, the data do not compare as well for RGM and PHg. Results showed a 2.7, 27 and 33% difference in the mean GEM, RGM and PHg concentrations, respectively, post QC of each program. It is recommended that RDMQ be used for data that is highly variable with high RGM/PHg concentrations as it allows for more manual correction over the QCed data. This investigation of 2 QC programs produced comparable data and that either of these programs can be used as standard methods for the quality control of atmospheric mercury speciation data.

Findings from quality assurance activities in the Integrated Atmospheric Deposition Network.

A series of experiments were conducted among the laboratories participating in the Integrated Atmospheric Deposition Network (IADN) monitoring program to evaluate comparability of the reported persistent organic pollutant concentrations. This quality assurance activity is essential because a variety of methods are currently used for sample collection, extraction, and analysis by the IADN laboratories. The experiments included analyses of a common reference standard (CRS), analyses of split samples, and analyses of samples collected with co-located samplers at the Point Petre IADN measurement station. The analytes included polycyclic aromatic hydrocarbons (PAHs), organochlorine pesticides (OCPs), and polychlorinated biphenyls (PCBs). For virtually all compounds, the laboratories produced generally comparable results for the CRS samples, the split samples and the co-location samples, although some differences were observed. Analysis of the methods may pinpoint areas where variations in the methods will result in the differences observed in the reported data. These differences can be due to the field sampling process, the analytical method, field blank values, or a combination of all these factors. This study points out the importance of QA activities at every step of an environmental monitoring process so that areas where improvements may be needed or where inconsistencies may exist can be identified.

Spatial patterns and temporal trends in mercury concentrations, precipitation depths, and mercury wet deposition in the North American Great Lakes region, 2002-2008.

Annual and weekly mercury (Hg) concentrations, precipitation depths, and Hg wet deposition in the Great Lakes region were analyzed by using data from 5 monitoring networks in the USA and Canada for a 2002-2008 study period. High-resolution maps of calculated annual data, 7-year mean data, and net interannual change for the study period were prepared to assess spatial patterns. Areas with 7-year mean annual Hg concentrations higher than the 12 ng per liter water-quality criterion were mapped in 4 states. Temporal trends in measured weekly data were determined statistically. Monitoring sites with significant 7-year trends in weekly Hg wet deposition were spatially separated and were not sites with trends in weekly Hg concentration. During 2002-2008, Hg wet deposition was found to be unchanged in the Great Lakes region and its subregions. Any small decreases in Hg concentration apparently were offset by increases in precipitation.

Pesticides in the atmosphere across Canadian agricultural regions.

The Canadian Atmospheric Network for Currently Used Pesticides (CANCUP) was the first comprehensive, nationwide air surveillance study of pesticides in Canada. This paper presentsthe atmospheric occurrence and distribution of pesticides including organochlorine pesticides (OCPs), organophosphate pesticides (OPPs), acid herbicides (AHs), and neutral herbicides (NHs) during the spring to summer of 2004 and 2005 across agricultural regions in Canada. Atmospheric concentrations of pesticides varied within years and time periods, and regional characteristics were observed including the following: (i) highest air concentrations of several herbicides (e.g., mecoprop, triallate, and ethalfluralin) were found at Bratt's Lake, SK, a site in the Canadian Prairies; (ii) the west-coast site at Abbotsford, BC, had the maximum concentrations of diazinon; (iii) the fruit and vegetable growing region in Vineland, ON, showed highest levels for several insecticides including chlorpyrifos, endosulfan, and azinphos-methyl; (iv) high concentrations of atrazine and metolachlor were measured at St. Anicet, QC, a corn-growing region; (v) the Kensington site in PEI, Canada's largest potato-producing province, exhibited highest level of dimethoate. Analysis of particle- and gas-phase fractions of air samples revealed that most pesticides including OCPs, OPPs, and NHs exist mainly in the gas phase, while AHs exhibit more diversity in particle-gas partitioning behavior. This study also demonstrated that stirred up soil dust does not account for pesticides that are detected in the particle phase. The estimated dry and wet deposition fluxes indicate considerable atmospheric inputs for some current-use pesticides (CUPs). This data set represents the first measurements for many pesticides in the atmosphere, precipitation, and soil for given agricultural regions across Canada.

Sources and occurrence of dacthal in the Canadian atmosphere.

Dacthal is a herbicide that can undergo long-range atmospheric transport. Due to limited use in Canada, its occurrence in the Canadian environment is likely associated with transboundary flow from the United States where 100 times more dacthal is used. To investigate its atmospheric distribution and possible sources, two sampling strategies were applied. First, polyurethane foam-disk passive air samplers were deployed across the country from the spring to summer of 2004 and 2005. Results showed highest dacthal concentrations at two sites in southern Ontario (max: 50 pg m(-3)) and much lower concentrations in other agricultural regions across Canada. Second, daily high-volume air samples were collected at a field site in north Toronto (Downsview). Sampling at this site was triggered by real-time meteorological forecast models that indicated when air flow to the site originated in the United States. Two such events, one in late June and one in late September 2005, were sampled. In both cases, elevated dacthal concentrations were captured (e.g., up to 319 pg m(-3) in the June event) and they were well correlated with transboundary flow from the United States. Finally, the octanol--air partition coefficient (K(OA)) of dacthal and other current-use pesticides was measured. K(OA) was used to derive a particle--gas partitioning coefficient (K(p)) for dacthal (Log K(p) = -4.1), indicating that this compound should exist mainly in the gas phase.

Temporal and spatial trends of atmospheric polychlorinated biphenyl concentrations near the Great Lakes.

Polychlorinated biphenyl (PCB) concentrations were measured in the atmosphere at six regionally representative sites near the five Great Lakes from 1990 to 2003 as part of the Integrated Atmospheric Deposition Network (IADN). Concentration data for several individual PCB congeners and for total PCBs were analyzed for temporal and spatial trends after correcting for the temperature dependency of the partial pressures. Atmospheric PCB concentrations are decreasing relatively slowly for tetra- and pentachlorinated congeners, an observation that is in agreement with primary emissions modeling. Relatively rapid decreases in PCB concentrations at the sites near Lakes Michigan and Ontario may reflect successful reduction efforts in Chicago and Toronto, respectively. Atmospheric PCB concentrations near Lakes Superior and Huron are now so low that the air and water concentrations may be close to equilibrium. Atmospheric PCB concentrations at sites near Lakes Michigan, Erie, and Ontario are relatively higher than those measured at sites near Lakes Superior and Huron. The highest PCB level was observed at the site near Lake Erie, most likely due to nearby urban activity. However, this relatively higher concentration is still 6-10 times lower than that previously reported at the Chicago site. A correlation between average gas-phase PCB concentration with local population indicates a strong urban source of PCBs. The temperature dependence of gas-phase PCB concentrations is similar at most sites except at Burnt Island on Lake Huron, where very low concentrations, approaching virtual elimination, prevent reliable temperature correlation calculations.

Atmospheric atrazine at Canadian IADN sites.

Atrazine is one of the most widely used herbicides in North America and has been primarily applied to corn production in the Great Lakes basin for over 30 years. During 1996-2002, atrazine concentrations in the atmospheric gas and particle phases were investigated at three Canadian Integrated Atmospheric Deposition Network (IADN) sites including two lakeside sites (Burnt Island and Point Petre) and a rural inland site (Egbert). Strong seasonality with peak concentrations occurring in late April-early July was observed. An atrazine usage map for Canada (sum: 870 t) and the United States (sum: 34 500 t) in 2002 was created. Local application and regional atmospheric transport both appear to contribute to its atmospheric occurrence, while the latter might episodically result in high concentrations events. No strong temperature dependence was observed for atrazine particle-gas partitioning. Recent measurement results of atrazine in precipitation samples collected at Egbert and another agricultural site, Vineland, through the Canadian Atmospheric Network for Currently Used Pesticides (CANCUP), are also presented, Dry, wet, and gas exchange deposition all contribute to atmospheric inputs of atrazine to the Great Lakes. For Lake Ontario, gas exchange is estimated to be of similar magnitude to dry and wet deposition.

Trends in polycyclic aromatic hydrocarbon concentrations in the great lakes atmosphere.

Atmospheric polycyclic aromatic hydrocarbon (PAHs) concentrations were measured in both the vapor and particle phases at seven sites near the Great Lakes as a part of the Integrated Atmospheric Deposition Network. Lower molecular weight PAHs, including fluorene, phenanthrene, fluoranthrene, and pyrene, were dominant in the vapor phase, and higher molecular weight PAHs, including chrysene, benzo[a]pyrene, and coronene, were dominant in the particle phase. The highest PAH concentrations in both the vapor and particle phases were observed in Chicago followed by the semiurban site at Sturgeon Point, NY. The spatial difference of PAH concentrations can be explained by the local population density. Long-term decreasing trends of most PAH concentrations were observed in both the vapor and particle phases at Chicago, with half-lives ranging from 3-10 years in the vapor phase and 5-15 years in the particle phase. At Eagle Harbor, Sleeping Bear Dunes, and Sturgeon Point, total PAH concentrations in the vapor phase showed significant, but slow, long-term decreasing trends. At the Sturgeon Point site, which was impacted by a nearby city, particle-phase PAH concentrations also declined. However, most particle-phase PAH concentrations did not show significant long-term decreasing trends at the remote sites. Seasonal trends were also observed for particle-phase PAH concentrations, which were higher in the winter and lower in the summer.

Polychlorinated naphthalenes in Great lakes air: assessing spatial trends and combustion inputs using PUF disk passive air samplers.

Passive air samplers made from polyurethane foam (PUF) disks housed in stainless steel chambers were deployed over four seasons during 2002-2003, at 15 sites in the Laurentian Great lakes, to assess spatial and temporal trends of polychlorinated naphthalenes (PCNs). Sampling rates, determined using depuration compounds pre-spiked into the PUF disk prior to exposure, were, on average, 2.9 +/- 1.1 m3 d(-1), consistent with previous studies employing these samplers. PCN air concentrations exhibited strong urban-rural differences-typically a few pg m(-3) at rural sites and an order of magnitude higher at urban sites (Toronto, 12-31 pg m(-3) and Chicago,13-52 pg m(-3)). The high concentrations at urban sites were attributed to continued emissions of historically used technical PCN. Contributions from combustion-derived PCNs seemed to be more important at rural locations where congeners 24 and 50, associated with wood and coal burning, were elevated. Congener 66/67, associated with incineration and other industrial thermal processes, was elevated at two sites and explained by nearby and/or upwind sources. Probability density maps were constructed for each site and for every integration period were shown to be a useful complement to seasonally integrated passive sampling data to resolve source-receptor relationship for PCNs and other pollutants.

Annual variation of polycyclic aromatic hydrocarbon concentrations in precipitation collected near the Great Lakes.

Polycyclic aromatic hydrocarbon (PAH) concentrations were measured in precipitation samples collected from 1997 to 2003 at seven sites near the Great Lakes as a part of the Integrated Atmospheric Deposition Network. The 28-day integrated concentrations of most PAHs showed significant seasonal trends with higher concentrations in the winter and lower concentrations in the summer. Long-term decreasing trends were observed for all PAHs measured in precipitation at Chicago. At the sites on Lakes Superior, Michigan,,and Erie, most PAHs did not show significant long-term trends. At the two Canadian sites on Lakes Huron and Ontario, lower molecular weight PAHs (e.g., fluorene to pyrene) showed long-term decreasing trends; however, no long-term trends were observed for higher molecular weight PAHs at these sites. Interestingly, retene, a marker for wood burning, showed increasing trends at the sites on Lakes Superior and Michigan. For all the other PAHs, precipitation collected at Chicago had by far the highest PAH concentrations followed by the site on Lake Erie. Generally, the Lake Superior sites had the lowest PAH concentrations. However, retene concentrations in precipitation collected at the Lake Superior site were higher compared to Lakes Michigan and Erie, which indicate more residential wood burning in the far north of the Great Lakes basin.

Temporal and spatial trends of organochlorine pesticides in Great Lakes precipitation.

Organochlorine pesticide concentrations in precipitation samples collected from 1997 to 2003 at seven Integrated Atmospheric Deposition Network sites around the Great Lakes are reported. The 28-day volume weighted mean concentrations of several pesticides, including gamma-hexachlorocyclohexane (HCH), endosulfan, hexachlorobenzene, chlordane, and DDE, showed significant seasonal trends. For current-use pesticides (endosulfan and gamma-HCH), their concentrations peaked in late spring to summer just after their agricultural application. For the banned pesticides, higher concentrations were observed in the winter due to their enhanced partitioning to particles and scavenging by snow. Long-term decreasing trends were observed for several pesticides such as gamma-HCH and DDE. On the other hand, beta-HCH showed significant increasing concentrations as a function of time at Brule River, Eagle Harbor, and Sleeping Bear Dunes. Generally, Chicago had the highest concentration of chlordanes, dieldrin, and DDT, indicating that urban areas could be a source for these compounds to precipitation. For gamma-HCH and endosulfans, Point Petre had the highest concentrations due to the application of these pesticides in the surrounding areas.

A comparison of European and North American atmospheric deposition networks: polycyclic aromatic hydrocarbons and lindane.

A comparison between the sampling and analytical methods used by Canadian (IADN) and German (OSPAR) regional monitoring networks for persistent organic pollutants was conducted from September 2002 to October 2003 at a rural site in Ontario, Canada. Polycyclic aromatic hydrocarbons (PAHs) and the currently-used pesticide lindane were measured in precipitation and ambient air samples. Overall the two networks sampling and analytical methods agreed well in their results of deposition (wet and dry particulate). Lindane concentrations between the two networks agreed well in the air samples while too few precipitation samples could be compared to conclude on agreement. The lindane seasonal profile with a peak in spring-early summer was consistent with previous results pointing to the continued use of this pesticide in 2002-2003 in Canada. Annual lindane wet depositions were comparable between the two network methodologies. PAHs concentrations in precipitation and in gas phase agreed well while there was a discrepancy for particulate PAHs in air. This study confirmed that the use of data from the two regional POPs monitoring networks for hemispherical modelling studies is warranted.

Spatial and seasonal variations of Hexachlorocyclohexanes (HCHs) and hexachlorobenzene (HCB) in the Arctic atmosphere.

Weekly high-volume air samples were collected between 2000 and 2003 at six Arctic sites, i.e., Alert, Kinngait, and Little Fox Lake (LFL) in Canada, Point Barrow in Alaska, Valkarkai in Russia, and Zeppelin in Norway. Hexachlorocyclohexanes (HCHs) and hexachlorobenzene (HCB) were quantified in all samples. Comparison showed that alpha-HCH and HCB were homogeneously distributed in the circumpolar atmosphere and uniform throughout the seasons. However, significantly higher atmospheric concentrations of alpha-HCH and HCB and strongertemperature dependence of alpha-HCH and gamma-HCH were found at LFL in Yukon (YK), which is unique among the sites by virtue of its high altitude and low latitude, resulting in higher precipitation rates and summer temperatures. Strong temperature dependence of alpha- and gamma-HCH at this location suggests that secondary emissions, i.e., re-evaporation from surfaces, were more important at this site than others. It is hypothesized that a higher precipitation rate at LFL facilitated the transfer of alpha-HCH from the atmosphere to surface media when technical HCH was still in use worldwide. On the other hand, higher temperature at LFL enhanced reevaporation to the atmosphere after the global ban of technical HCH. In contrast to alpha-HCH and HCB, larger spatial and seasonal differences were seen for gamma-HCH (a currently used pesticide), which likely reflect the influence of different primary contaminant sources on different Arctic locations. Fugacity ratios suggest a net deposition potential of HCB from air to seawater, whereas seawater/air exchange direction of alpha-HCH varies in the circumpolar environment.

Resolving the long-term trends of polycyclic aromatic hydrocarbons in the Canadian Arctic atmosphere.

Polycyclic aromatic hydrocarbon (PAH) air concentrations measured over the period 1992-2000 at the Canadian High Arctic station of Alert were subject to time-series analysis using dynamic harmonic regression (DHR). For most of the PAHs, the DHR model fit to the observed data was good, with DHR capable of interpolating over missing data points during periods when air concentrations were below detection limits. As expected, DHR identified seasonal increases in PAH air concentrations. However, it has also identified additional, subtler "seasonal" patterns as a series of harmonics with varying periodicity. For example, a regular summer high in air concentrations was apparent for many PAHs, particularly the lower molecular weight (two- to three-ringed) compounds, which may be attributed to summertime regional combustion events such as forestfires and/or revolatilization from surfaces (e.g., soil and oceans, as well as arctic surfaces). Comparison of wintertime PAH concentrations (where sigmaPAH ranged from 260 to 516 pg m(-3)) with an earlier arctic study did not reveal a reduction in PAH levels. However, removal of the seasonal components by DHR revealed a declining trend in PAH concentrations over the 1992-2000 period. For many lighter PAHs, this was typified by a linear decrease over the whole time series, although, for the higher molecular weight PAHs, a marked reduction was apparent in the first few years of sampling followed by a leveling off in concentrations by the mid/late-1990s. This behavior is similar to reported trends of other air pollutants in the Arctic, may be attributed to the decline in Soviet industry during the early 1990s, and has implications regarding the major PAH sources affecting the Arctic.

How do climate fluctuations affect persistent organic pollutant distribution in North America? Evidence from a decade of air monitoring.

Interannual variations of persistent organic pollutant (POP) air concentrations from the Great Lakes region and the Arctic during the 1990s are strongly associated with atmospheric low-frequency fluctuations, notably the North Atlantic Oscillation (NAO), the El Niño-Southern Oscillation (ENSO), and the Pacific North American (PNA) pattern. This suggests interactions between climate variation and the global distribution of POPs. Atmospheric concentrations of hexachlorocyclohexanes (HCHs), hexachlorobenzene (HCB), and several lighter polychlorinated biphenyls (PCBs) measured around the Great Lakes basin increased during the positive phases of NAO and ENSO in the spring. This implies that anomalous high air temperatures associated with NAO and ENSO enhance volatilization of POPs from reservoirs on the Earth's surface accumulated in the past. These compounds are then available for transport from source regions to more pristine regions such as the Arctic under favorable flow patterns associated with global climate variations.

Impacts of lindane usage in the Canadian Prairies on the Great Lakes ecosystem. 2. Modeled fluxes and loadings to the Great Lakes.

Atmospheric loadings of gamma-hexachlorocyclohexane (gamma-HCH) from May 1, 1998, to April 30, 1999, to the Great Lakes simulated by a coupled soil-air and water-air atmospheric transport model are presented. Modeling results on an annual basis indicate that Lake Superior received the highest dry deposition load of 2.17 kg yr(-1). Dry deposition to the lower Great Lakes (Lakes Erie and Ontario) was 2-6 times lower as compared to the upper Great Lakes. Greater deposition in the upper Great Lakes is due mainly to their larger surface area and greater proximity to sources of gamma-HCH. Dry deposition fluxes (pg m(-2)) to lake surfaces were much lower than to land as a result of lower deposition velocities and lower air concentrations of gamma-HCH over the lakes. The highest gamma-HCH loading (kg yr(-1), in 1998-99) due to wet deposition occurred for Lake Ontario. This was mainly attributed to greater annual rainfall over Lake Ontario. An investigation of average seasonal fluxes predicted by the model shows that deposition fluxes to the Great Lakes are considerably higher in the summer than that in the autumn and winter seasons. The net direction of gas exchange also exhibits a seasonal dependence. Lakes Michigan, Huron, and Ontario show net absorption in the summer 1998 whereas at all other times net outgassing occurred at all of the lakes. Overall, gas exchange was the dominant process affecting loadings to the Great Lakes. Model-derived loadings and total deposition flows across the Great Lakes basin due to dry and wet depositions and net gas exchange agree reasonably well with the summer estimates compiled by the Integrated Atmospheric Deposition Network whereas autumn values show greater discrepancies. Better agreement was also observed for dry deposition as compared to wet deposition. Specifically, to improve short-term loading estimates (e.g., over days to months), the model results indicate the need for better spatially and temporally resolved information on concentrations in air and surface water and better estimates of precipitation and deposition velocities over the lakes.