Single crystals of (Ca1-xSrx)(2)MgSi2O7 slightly doped with 1000 ppm Mn2+ a
nd with x ranging from 0.04 to 0.32 were grown from the melt in a mirror fu
rnace applying the Czochalski technique. Transmission electron microscopy (
TEM) revealed incommensurately modulated structures at room-temperature for
all compositions in accordance with earlier studies by electron paramagnet
ic resonance (EPR). Electron diffraction patterns clearly show satellite re
flections typical for two-dimensional modulation, and their successive dest
abilization with increasing Sr content. The modulation is of tartan-like ap
pearance. Beyond a Sr/(Sr+Ca) ratio of about 0.32 the synthesis of stable s
olid solution akermanite type crystals was proved not to be feasible, indic
ating the existence of a miscibility gap in the Sr akermanite system. As pr
esumed from the diffuse scattering around the satellite reflections, and su
ggested more conclusively by crystallographic processing of high resolution
EM images the Sr ions incorporated into the incommensurate crystal phase a
re distributed in an ordered fashion and are partly adapted to the displaci
ve modulation of the pure akermanite. This means, occupational modulation e
ven makes a contribution to the overall modulation characteristics in (Ca1-
xSrx)(2) MgSi2O7.