Hehh, I'm in a VMware class right now, but I've been doing it a couple years. What you're looking for is "extents".
Basically lets say you have 4tb of unused space in multiple LUNs. Make an initial datastore using all the space on LUN 1. Then select that new datastore in the datastore and datastore clusters view. Select Configuration -> Properties. Click Increase, and it should give you the unused LUNs to add to this initial datastore.
In your case, whack an unused LUN or get a new one. Then just do the Increase on the existing DS...





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