From 1974-2014 Yakutsk data, the rate of change of air shower maximum with energy is nonlinear, indicating a changing cosmic ray mass composition over 10^16 to 5.7x10^19 eV.
Greisen, Physical Review Letters 16, 748 (1966)
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Mass composition of cosmic rays above 0.1 EeV by the Yakutsk array data
From 1974-2014 Yakutsk data, the rate of change of air shower maximum with energy is nonlinear, indicating a changing cosmic ray mass composition over 10^16 to 5.7x10^19 eV.