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The energy distributions of liquid metal ion sources using Au–Si–Be, Pd–Ni–Si–Be–B, Al–Si, and Pt–Si alloys have been measured. Profiles of singly charged ion species which are strongly dependent on alloy systems typically exhibit an abrupt rise at the high‐energy position and gradual decay at the low‐energy position in the profiles. This gradual decay, which appears rather like a subsidiary shoulder, may be caused by free space field ionization in addition to field evaporation. Profiles also have long tails at both the high‐ and low‐energy positions. These tails can be explained by charge transfer collision between ions and neutral atoms coming from the outer space. The intensity of the tails is discussed on the basis of the charge transfer collision process.