Book excerpt: Radionuclide contamination in the soil and groundwater at U.S. Department of Energy (DOE) sites is a severe problem requiring monitoring and remediation. Radionuclide measurement techniques are needed to monitor surface waters, groundwater, and process waters. Typically, water samples are collected and transported to the analytical laboratory where costly radiochemical analyses are performed. To date, there has been very little development of selective radionuclide sensors for alpha- and beta-emitting radionuclides such as 9°Sr, 99Tc, and various actinides of interest. The objective of this project is to investigate novel sensor concepts and materials for sensitive and selective determination of beta- and alpha-emitting radionuclide contaminants in water. To meet the requirements for low-level, isotope-specific detection, the proposed sensors are based on radiometric detection. As a means to address the fundamental challenge of short ranges of beta and alpha particles in water, our overall approach is based on localization of preconcentration/separation chemistries directly on or within the active area of a radioactivity detector, using automated microfluidics for sample manipulation and sensor regeneration or renewal. The outcome of these investigations will be the knowledge necessary to choose appropriate chemistries for selective preconcentration of radionuclides from environmental samples, new materials that combine chemical selectivity with scintillating properties, new materials that add chemical selectivity to solid-state diode detectors, new preconcentrating column sensors, and improved instrumentation and signal processing for selective radionuclide sensors. New knowledge will provide the basis for designing effective probes and instrumentation for field analytical chemistry.