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Illite crystals in siliciclastic sediments are heterogeneous assemblages of detrital material coming from various source rocks and, at paleotemperatures &gt;70 °C, of superimposed diagenetic modification in the parent sediment. We distinguished the relative proportions of 2M 1  detrital illite and possible diagenetic 1M d  + 1M illite by a combined analysis of crystal-size distribution and illite polytype quantification. We found that the proportions of 1M d  + 1M and 2M 1  illite could be determined from crystallite thickness measurements (BWA method, using the MudMaster program) by unmixing measured crystallite thickness distributions using theoretical and calculated log-normal and/or asymptotic distributions. The end-member components that we used to unmix the measured distributions were three asymptotic-shaped distributions (assumed to be the diagenetic component of the mixture, the 1M d  + 1M polytypes) calculated using the Galoper program (Phase A was simulated using 500 crystals per cycle of nucleation and growth, Phase B = 333/cycle, and Phase C = 250/cycle), and one theoretical log-normal distribution (Phase D, assumed to approximate the detrital 2M 1  component of the mixture). In addition, quantitative polytype analysis was carried out using the RockJock software for comparison. The two techniques gave comparable results (r 2  = 0.93), which indicates that the unmixing method permits one to calculate the proportion of illite polytypes and, therefore, the proportion of 2M 1  detrital illite, from crystallite thickness measurements. The overall illite crystallite thicknesses in the samples were found to be a function of the relative proportions of thick 2M 1  and thin 1M d  + 1M illite. The percentage of illite layers in I-S mixed layers correlates with the mean crystallite thickness of the 1M d  + 1M polytypes, indicating that these polytypes, rather than the 2M 1  polytype, participate in I-S mixed layering.

Detrital illite crystals identified from crystallite thickness measurements in siliciclastic sediments