Chapter 2 U- and Th-Series Nuclides in the Atmosphere: Supply, Exchange, Scavenging, and Applications to Aquatic Processes

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This chapter summarizes the use of U- and Th-series nuclides particularly 222Rn and its daughter products in the study of scavenging processes in the atmosphere. The chapter also includes progress made in these fields during recent years, as well as perspectives on their use in aquatic systems. 238U and 232Th are primordial radionuclides contained in rocks and minerals. Other sources of U- and Th-series nuclides to the atmosphere include volatile emissions from biogenic sources, and anthropogenic activities such as fossil fuel combustion, depleted uranium from military activities, sewage digestion, landfills, and mining activities. The distribution of U- and Th-series nuclides in the atmosphere is governed by their supply, atmospheric circulation/mixing, removal by scavenging/deposition and radioactive decay. The scavenging of nuclides from the atmosphere and their subsequent deposition on Earth's surface are important processes governing their supply to lakes and ocean surface waters and provides the basis for their applications as tracers to investigate selected processes in these reservoirs. The atmospheric deposition flux of 210Pb and other nuclides can be determined directly or by sampling natural collectors. Among the U-series nuclides of atmospheric origin, 210Pb has found extensive applications to determine chronologies of a variety of aqueous system deposits and thereby provide a time frame for records stored in them. The generation of 210Pb in the atmosphere from its gaseous grandparent 222Rn has led to many uses in tracing the transport and scavenging of similarly generated elements. Another application of 210Pb has been to track the deposition of trace metals from the atmosphere to the sea surface. However, these applications require a large number of nuclide measurements, specifically high-resolution spatial and temporal measurements of 222Rn and its daughters in the atmosphere. Recent studies should enhance the use of U-series nuclides as tracers of atmospheric and their subsequent aquatic processes.

Introduction

The atmosphere is an important pathway for the exchange and transfer of selected U- and Th-series nuclides between land and various aquatic reservoirs. This makes the study of the atmospheric supply of these U- and Th-series nuclides, and their distribution and removal from the atmosphere, important to investigate various aquatic processes. This is particularly relevant for the latter part of the 238U-series, the so-called radon (222Rn)-daughter series with prominent atmospherically derived progeny (Figure A1). These radionuclides are useful in quantifying the rates of both atmospheric and aquatic processes, such as gas and particulate exchange, mixing, scavenging and sedimentation. In addition, the U- and Th-series nuclides can also serve as tracers of aerosol provenances and can help track their atmospheric trajectories and sources to aquatic systems.

This chapter builds on two comprehensive reviews on atmospheric 222Rn and daughter products (Turekian et al., 1977) and natural radionuclides in the atmosphere (Turekian and Graustein, 2003). Here we include progress made in these fields during recent years, as well as perspectives on their use in aquatic systems. Thus the scope of the chapter includes the use of U- and Th-series nuclides particularly 222Rn and its daughter products in the study of scavenging processes in the atmosphere, gas exchange/transfer across the air–water interface and particle-associated processes in selected reservoirs of the hydrosphere, such as snow/ice, lakes and coastal ocean. This chapter is complementary to the chapters by Chabaux et al. dealing with freshwater processes, Rutgers van der Loeff and Geibert on scavenging processes in seawater, Chase on sedimentary processes, Stewart et al. on bioaccumulation of U–Th nuclides, and McKee dealing with estuarine processes.

Section snippets

Sources of U- and Th-Series Nuclides to the Atmosphere

The 238U- and 232Th-series nuclides are introduced into the atmosphere primarily through the following pathways.

Atmospheric Distributions

The distribution of U- and Th-series nuclides in the atmosphere is governed by their supply, atmospheric circulation/mixing, removal by scavenging/deposition and radioactive decay. The supply, as mentioned in Section 2, is dominated by continental sources and in situ production in the atmosphere.

Aerosol Scavenging Residence Times Using 222Rn and Its Daughters

The 222Rn daughters (210Pb, 210Bi and 210Po) interact with aerosols leading to their differential scavenging depending on their respective chemistry. This differential removal of nuclides in this sub-series provides an approach to estimate their atmospheric residence times, those of their chemical homologues and of the fine particles with which they associate (Poet et al., 1972; Moore et al., 1973; Martell and Moore, 1974). The residence times can be derived based on models of different

Sedimentation and trace element accumulation

Among the U-series nuclides of atmospheric origin, 210Pb has found extensive applications to determine chronologies of a variety of aqueous system deposits and thereby provide a time frame for records stored in them. 210Pb has been successfully used to date sediments from lakes and coastal ocean, marshes, coastal bays and shelf and snow. The principles of the 210Pb method are presented in detail in Krishnaswami and Lal (1978), with applications reviewed in Appleby and Oldfield (1992), and

Radon exchange models across the air–sea interface

The 222Rn produced from dissolved 226Ra in surface seawater escapes to the atmosphere as the air over the ocean is essentially devoid of 222Rn, and such escape of 222Rn causes 222Rn-226Ra disequilibrium (Figure 2). The nature and extent of the 222Rn-226Ra disequilibrium have been used to derive air–water gas exchange parameters (Broecker and Peng, 1971, Broecker and Peng, 1974, Broecker and Peng, 1982; Cochran, 1992).

The basis for estimating evasion of gases from the surface ocean to the

Perspectives and Future Directions

Since the work of Moore et al., 1973, Moore et al., 1974, atmospheric radon and its progenies have been used widely to tag aerosols and time their scavenging process in the atmosphere. These applications were a direct result of efforts to understand the transport and fate of nuclear weapon debris in the atmosphere and provided some of the key results on the mixing proportions and residence times of atmospheric aerosols. Since then, the scope of applications using these nuclides has been

Acknowledgements

The genesis of this review was made possible during a study fellowship visit awarded to TMC by the Hanse Wissenshaftskolleg, Delmenhorst, Germany, during the spring of 2006. We acknowledge Dr R. Rengarajan for his help in providing experimental details and additional references. We also acknowledge the thorough assistance from the Editor S. Krishnaswami in a more substantial compilation of the manuscript, and the comprehensive and sage editorial advice from Editor J. K. Cochran.

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