Spatial and Temporal Variations in CHLORINE-36 Deposition in the Northern United States

Chlorine-36, a cosmogenic radioisotope, has been developed for use as a tracer in hydrological systems. The deposition of atmospheric ^{36} Cl, although of primary importance to hydrological applications, has not been well studied. To begin to address this problem, ^{36}Cl has been measured in monthly, wet-only, precipitation samples collected from February, 1991, to January, 1993, at the Elms Environmental Education Center in St. Mary's County, Maryland. In addition, bulk deposition samples were collected over a 1 y period at seven sites across the Northern United States and analyzed for ^{36} Cl. The mean, wet-only ^{36} Cl/Cl ratio for the 2 y sampling period is 68 +/- 19 (x10^{-15} ) and the mean ^{36}Cl concentration is 1.2 +/- 0.1 (x10 ^6) atoms/L. The ^ {36}Cl wet deposition flux data reveal a distinct seasonal deposition pattern, with peaks occurring in March and April. This pattern is attributed to stratospheric/tropospheric exchange. The mean ^{36}Cl wet deposition flux is 38.2 +/- 5 atoms/m^2s. Comparison between wet-only and bulk deposition samples indicates that the difference accounts for approximately 25% of the total ^{36}Cl deposition flux at the Elms site. A new model, using ^{90} Sr to predict the ^{36} Cl deposition pattern, is developed to predict ^{36}Cl/Cl ratios across the United States. Chlorine-36/Cl ratios in bulk deposition samples collected across the northern United States agree well with the model predictions. A mean global ^{36}Cl production rate of approximately 28 to 38 atoms/m^2s is indicated by these samples. A comparison between ^{36 }Cl concentrations in the Aquia and Magothy aquifers in southern Maryland and bulk deposition samples collected at the Elms, MD, site indicated that modern precipitation can account for the ^{36}Cl content in the youngest water in these aquifers. Surface water samples from the Susquehanna River basin reveal ^{36}Cl and stable chloride concentrations an order of magnitude higher than in bulk deposition samples collected at State College, PA. The source of excess ^{36}Cl in the Susquehanna is not known. Possible explanations include 'bomb-pulse' ^{36}Cl and in-situ ^{36}Cl production in surface rocks.