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Using high-resolution visible and near-infrared diffuse spectral reflectance, we have systematically investigated apparent wavelength shifts as a function of mineral chemistry in the Fe/Mg olivine series from Fo11 to Fo91. The study also shows that trace amounts of nickel can be spectrally detected in the olivine structure. We show that significant compositional information can only be extracted at relatively high resolution, because the overall spectral characteristics of the olivines change only subtly as a function of the Fe/Mg ratio. Significant spectral variation as a function of grain size is also demonstrated, adding a further complication to the interpretation of remotely sensed data from olivine-rich surfaces. This laboratory study is expected to aid in the interpretation of remotely sensed data from both terrestrial and extraterrestrial bodies. Terrestrial applications may include the recognition of ultramafic, ultrabasic, and basaltic terrains which in themselves may have mineral potential. Among extraterrestrial applications, the asteroids are obvious candidates for further examination if instrumentation can provide the necessary wavelength coverage, resolution, and signal-to-noise ratio so that spectra can be compared to those laboratory data discussed here. Some permutations of Fe-Mg-Ni relations in olivines are discussed as they apply to the interpretation of asteroid surfaces and other extraterrestrial bodies.