PNL-7487 UC-603 encouragement and support, Robert Turner and Craig Brandt of Oak Ridge National Laboratory for assistance in data analysis, S. S. Dixit and B. F. Cumming of Queen's University for providing unpublished data; and E. C. Krug of the Illinois State Water Survey for his detailed critique of the report. This research would not have been possible without the considerable efforts of Robbins Church and coworkers in the Direct Delayed Response Project and of John Smol and coworkers in the PIRLA-11 project • iii Thirty-three lakes that had been statistically selected as part of the U.S. Environmental Protection Agency's Eastern Lake Survey and Direct Delayed Response Project (DDRP) were used to compare the MAGIC (watershed) and Diatom (paleolimnological) models. The study lakes represented a well-defined group of Adirondack lakes, each larger than 4 ha in area and having acidneutralizing capacity (ANC) < 400 ~eq L•'. The study first compared current and pre-industrial (before !850) pH and ANC estimates from Diatom and MAGIC as they were calibrated in the preceding Paleocological Investigation of Recent Lake Acidification (PIRLA) and DDRP studies, respectively. Initially, the comparison of hindcasts of pre-industrial chemistry was confounded by seasonal and methodological differences in lake chemistry data used in calibration of the models. Although certain differences proved to be of little significance for comparison, MAGIC did predict significantly higher pre-industrial ANC and pH values than did Diatom, using calibrations in the preceding studies. To remove known calibration biases, both models were recalibrated for selected scenarios. The more realistic pre-industrial sulfur deposition level (~13% of 1984 value) in the recalibrated MAGIC scenario reduced the hindcast ANC values significantly, reducing the discrepancy between the two models and indicating the sensitivity of process-level watershed models to assumptions concerning the quantity of atmospheric deposition. The reaggregation to subregional soils data appeared to produce little effect on hindcast ANC and pH values. A recalibrated MAGIC scenario using reaggregated soils data, sulfate loss-tolake sediment, and partial pressure of C0 2 specific to the Adirondack subregion, was also compared to a Diatom scenario using a similar sum of base cations minus sum of strong acid anions definition of ANC. The result yielded MAGIC hindcasts closer to Diatom hindcasts, but still significantly higher pre-industrial ANC and pH values than suggested by the Diatom model. Both models suggest acidification of low ANC Adirondack region lakes since preindustrial times, but differ primarily in that MAGIC inferred greater acidification and that acidification has occurred in all lakes in the comparison, whereas Diatom inferred that acidification has been restricted to low ANC lakes (