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Step 1. Build Ni(CO)4

The stucture is perfectly tetrahedral. You should be able to build the molecule yourself, using the techniques described in earlier tutorials. One possible way:

Start ADFinput
Build a tetrahedral metal complex using the Structures button
  (Metal Complexes>ML4 tetrahedral) 
Change the central atom into a Ni atom
Select the ligands (use the pop-up menu Atom Popup → Select All XX atoms)
Change them in CO ligands (again in the pop-up menu Atom Popup → Add Structures → Ligands → CO)
Choose the 'Geometry Optimization' Preset
Save and Run
When the run has finished, click 'yes' to import the optimized coordinates
Save 

Your molecule should look something like this:

NiCO4 molecule

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