Direct Fabrication of Large Micropatterned Single Crystals Joanna Aizenberg, David A. Muller, John L. Grazul, and D. R. Hamann

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Fig. S1: Transmission electron diffraction patterns showing the film microstructure. (A) Diffraction pattern of the as deposited material shows only the diffuse scattering characteristic of an amorphous material. (B) The final calcite film has a crystalline diffraction pattern. Images recorded in a JEOL 2010F TEM in scanning- TEM mode with a 3mrad convergence angle and 5 pA of beam current to minimize sample charging, which occurred when operated with the higher beam currents of TEM mode. (C) TEM image of a sample calcite section and electron diffraction pattern from the entire region. Shards of the crystal were cross-sectioned by ultramicrotoming to produce 70-nm-thick electron transparent sections. Operating the microscope at low magnifications (2000x), we were able to obtain diffraction patterns from crystal sections as large as 50 m². The electron diffraction from these sections shows a single-crystal pattern. Dark-field images in diffracted beams revealed that the entire region diffracted uniformly, i.e. no amorphous or small polycrystalline inclusions were detected.

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• Movie S1
  Crystal formation was monitored in real time by optical microscopy. All images, except for the 1^st frame, were recorded in the transmission mode under polarized light. Frames were collected every 2 min. The scale and time are shown. Arrows indicate defects in the original film at which pinning of the crystallization front occurs. In the experiment shown, the micropattern consisted of a square array of 5 m posts separated by 10 m spaces.

• Movie S2
  Micropatterned crystal rotated under polarized light.