The time files due to radioactive decay events were analyzed for the selective extraction of successive alpha-decay pulse events in millisecond orders, such as216Po (145 ms, thorium series),217At (32.3 ms, neptunium series), and215Po (1.78 ms, actinium series) after respective preceding parents decay, using a multiple time interval analysis (TIA-MTA) technique from both theoretical and experimental viewpoints. In the theoretical treatments, the detection sensitivities of each correlated event in natural decay series was compared with more generalized conditions. It was noteworthy that the evaluated detection sensitivity had increased proportionally with shorter half-lives in the following order:214Po>215Po>217At>216Po.Finally, the present TIA was applied to the clarification of thorium series disequilibrium states in Tamagawa (Akita, Japan) Hot Spring waters. Activities of224Ra were evaluated to be 3.41±0.38 and 0.60±0.08 Bq/l at the upper and lower stream, respectively. The results from activity ratios of radium to thorium isotopes showed a preferential precipitation of radium isotopes in comparison with thorium, reflecting the sensitivity to the lowering acidity of strongly acidic hot spring waters in the lower end of the stream.