Single-, double-, and triple resonance excitation schemes, using extended-cavity and frequency-doubled diode lasers, have been investigated for highly selective RIMS detection of calcium isotopes. The single-resonance scheme has been applied to isotope ratio measurements in blood serum and meteorite samples. The double- and triple-resonance schemes have been evaluated for improvements in selectivity and sensitivity, with a goal of providing overall isotopic selectivity > 10(15) for radiochemical dating measurements with Ca-41.