Detection of leakage in deep geologic storage formations (e.g., carbon sequestration sites) is a challenging problem. This study investigates an easy-to-implement frequency domain leakage detection technology based on harmonic pulse testing (HPT). Unlike conventional constant-rate pressure interference tests, HPT stimulates a reservoir using periodic injection rates. The fundamental principle underlying HPTbased leakage detection is that leakage modifies a storage system's frequency response function, thus providing clues of system malfunction. During operations, routine HPTs can be conducted at multiple pulsing frequencies to obtain experimental frequency response functions, using which the possible time-lapse changes are examined. In this work, a set of analytical frequency response solutions is derived for predicting system responses with and without leaks for single-phase flow systems. Sensitivity studies show that HPT can effectively reveal the presence of leaks. A search procedure is then prescribed for locating the actual leaks using amplitude and phase information obtained from HPT, and the resulting optimization problem is solved using the genetic algorithm. For multiphase flows, the applicability of HPT-based leakage detection procedure is exemplified numerically using a carbon sequestration problem. Results show that the detection procedure is applicable if the average reservoir conditions in the testing zone stay relatively constant during the tests, which is a working assumption under many other interpretation methods for pressure interference tests. HPT is a cost-effective tool that only requires periodic modification of the nominal injection rate. Thus it can be incorporated into existing monitoring plans with little additional investment.