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Is it possible to assign a new unicode to a new character in Fontlab?
For me, anyway, your question isn't clear. Do you mean "create" a new Unicode number, such as F0000? No, you can't do that, just like you couldn't create a "new" ASCII character -- a standard is just that. The only exception is private use Unicode numbers, already provided for in the standard, such as E100 etc.
But if you mean assign (correctly) an existing Unicode number, sure, just as you would assign a new name. On the PC, the window comes up using "alt+G+R" (alt glyph rename).