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We use a genetic algorithm (GA) to optimize the mass resolution and detection efficiency of a multi-photon ionization, time-of-flight mass spectrometer. The algorithm uses experimental fitness functions to optimize eight voltages supplied to a set of ion optics. The GA optimized the ion detection efficiency by a factor of 10 and the mass resolution by a factor of 11 over previous settings obtained from computer simulations of the instrument. This experiment highlights the usefulness of adaptive algorithms to the experimental optimization of multidimensional search problems commonly found in modern laboratories. © 1999 American Institute of Physics.