Interpretation of mullite HREM images along [010] and [100]

200 kV and 300 kV HREM images of mullite with beam direction parallel to 010] and 100] have been compared with extensive multi-slice calculations of structure models with different oxygen vacancy arrangements. The simulations reveal that changes of the contrast pattern in HREM images are correlated with enhanced vacancy concentrations and coupled cation shifts (Al^*). Furthermore, the direct relationship between contrast variation and projected vacancy concentration permits the detection of 20% oxygen vacancies along 010] and 100]. An analysis of HREM images indicates preferred orientations of vacancies parallel to 〈102〉 in the (010) plane, whereas the (010) plane yields arrangements parallel to 〈012〉 and 〈001〉, resulting in an average direction of 〈013〉. Distances of 1.5a and 1.5b between these arrangements result from preferred inter-vacancy correlation vectors of 1/2 〈310〉 and 1/2 〈130〉 in the (001) plane. The investigated 2:1 and 3:2-mullites (x = 0.40 and x = 0.25) do not show long-range ordered arrangements of oxygen vacancies, but reveal the composition-dependent formation of short-range order regions of enhanced vacancy concentrations. These regions are distributed in a matrix with a minor degree of order.