High-speed digital imaging has been used in rapid compression facility (RCF) studies to investigate ignition phenomena of iso-octane/air mixtures. Sequential images were captured for each experiment. The results indicate the existence of two ignition regimes. In one domain, ignition is rapid, typically less than 76 mu s, and ignition occurs simultaneously throughout the test volume. In the other domain, reaction fronts form and propagate within the test volume prior to volumetric ignition. The data span equivalence ratios from phi = 0.20 to 1.98, with inert/O-2 gas ratios from 1.38 to 5.89, pressures from 8.7 to 16.6 atm, and temperatures from 903 to 1020 K. The transition between the two regimes is discussed in the context of the mixture composition and experimental conditions. The analysis shows that the fuel mole fraction is a key parameter dictating the boundary between the modes of ignition. Below a critical mole fraction limit, volumetric ignition is observed; above the critical limit, reaction fronts are consistently present prior to volumetric ignition. The ignition delay times for both ignition regimes are well reproduced using a homogeneous simulation with detailed reaction chemistry, when the state conditions are modified to account for the presence of the reaction fronts. The results are discussed in terms of proposed reaction chemistry, ignition theory, and previous studies of iso-octane ignition. (c) 2006 The Combustion Institute. Published by Elsevier Inc. All rights reserved.