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The authors tested the theory that hemispheric specialization evolved as a consequence of reduced interhemispheric connectivity by examining whether neuroanatomical asymmetries were associated with variation in the ratio of corpus callosum size to brain volume (CC:VOL) and to neocortical surface area (CC:NEO) in human and nonhuman primates. Magnetic resonance images were collected in a sample of 45 primates including 8 New World monkeys, 10 Old World monkeys, 4 lesser apes, 17 great apes, and 6 humans. CC:VOL and CC:NEO were determined and correlated with measures of brain asymmetry. The results indicate that brain asymmetry significantly predicted CC:VOL and CC:NEO. Subsequent analyses revealed that species variation in functional asymmetries in the form of handedness are also inversely related to CC:NEO. Taken together, these results support the hypothesis that leftward brain asymmetries may have evolved as a consequence of reduced interhemispheric connectivity.