What physical limitation ultimately caused the vacuum brake to decline in favor of high-pressure air systems for heavy, fast trains?

Answer

It required a very large brake piston and cylinder for a given stopping force.

Because the stopping force in a vacuum system depends on the atmospheric pressure differential (maxing out around 30 inHg), it needed much larger brake pistons and cylinders compared to high-pressure air systems to generate equivalent stopping force.

What physical limitation ultimately caused the vacuum brake to decline in favor of high-pressure air systems for heavy, fast trains?
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