The structural analysis of crystal defects in organic thin films provides fundamental insights into their electronic properties for applications such as field effect transistors. Observation of crystal defects in organic thin films has previously been performed at rather low resolution by conventional transmission electron microscopy based on phase-contrast imaging. Herein, we apply for the first time annular dark-field imaging to the direct observation of grain boundaries in copper hexachlorophthalocyanine thin films at the atomic resolution level by using an aberration-corrected scanning transmission electron microscope combined with electron energy-loss spectroscopy. By using a low-dose technique and an optimized detection angle, we were able to visualize the contrast of light element (C and N) together with the heavier elements (Cl and Cu) within the molecular column. We were also able to identify unexpected molecular orientations in the grain boundaries along the {110} crystallographic planes giving rise to stacking faults.

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