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3 to the chest and 1 to the head is a better option as shooting at the chest, which is obviously the larger target, for the first 3 shots minimises the chances of any of the bullets missing due to the spread etc and all the bullets need to connect to put the player one shot for the 4th shot.
Also, as it doesn't matter where the first three shots hit as they take the shield down regardless, you're just making it harder on yourself by trying to aim for the head when any part of the body will do.