Why did the balloons get bigger when the pump was turned on?
Because as the pump sucks the air out around the balloons they had to fill the empty space and thus expanded.
What was happening at the molecular level?
The molecules on the outside that were getting taken away are why the balloons expanded. They molecules outside the balloon kept bouncing into and away from the balloon, but once you start to remove the molecules around the balloon it has nothing holding it in. Once there is no molecules around the balloon bouncing against it it expands.
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