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Process models are widely used tools, both for studying fundamental processes themselves and as elements of larger system studies. A radiative transfer model (RTM) simulates the interaction of light with a medium. We are interested in RTMs that model light reflected from a vegetated region. Such an RTM takes as input various biospheric and illumination parameters and computes the upwelling radiation at the top of the canopy. The question we address is as follows: Which of the inputs to the RTM has the greatest impact on the computed observation? We study the leaf canopy model (LCM) RTM, which was designed to study the feasibility of observing leaf chemistry remotely. Its inputs are leaf chemistry variables (chlorophyll, water, lignin, and cellulose) and canopy structural parameters (leaf area index, leaf angle distribution, soil reflectance, and sun angle). We present a statistical approach to the sensitivity analysis of RTMs to answer the question previously posed. The focus is on global sensitivity analysis, studying how the RTM output changes as the inputs vary continuously according to a probability distribution over the input space. The influence of each input variable is captured through the ldquomain effectsrdquo and ldquosensitivity indices.rdquo Direct computation requires extensive computationally expensive runs of the RTM. We develop a Gaussian process approximation to the RTM output to enable efficient computation. We illustrate how the approach can effectively determine the inputs that are vital for accurate prediction. The methods are applied to the LCM with seven inputs and output obtained at eight wavelengths associated with Moderate-resolution Imaging Spectroradiometer bands that are sensitive to vegetation.