Over volting..

In a word yes but you don't do it with voltage on LED's you up the current. LED's require a constant current, so if you want it brighter you up the current doing it using the voltage will just lead to them going pop, as the led gets hotter the current flow will remain the same but the Vf will decrease so if you were regulating the voltage and kept it the same as the led got hotter the current would climb and lead to thermal runaway.

The drgree to which an led can be over run depends on how good your heatsink is. Have a look at this light i made as an example of how much heatsinking might be required http://www.candlepowerforums.com/vb/showthread.php?t=214001
 
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