At these pressures, and assuming that the temperature is 72F, you can safely assume that the ideal gas law applies and it becomes a very simple calculation.
The basic equation is PV = nRT
i.e. the product of absolute pressure and volume equals the product of the number of moles of gas present, the universal gas constant and the absolute temperature.
If the pressure is psia, the volume is US gallon, n is lb mole and temperature is Rankine then R is 80.278 (from Uconeer).
We want to calculate the amount of gas present so we re-arrange the formula to give
n = (PV)/(RT) , and note that V, R and T are constants so we have
n = (P x 30) / (80.278 x 531.67) = P x 0.0007029
When the evacuated tank is pressurized to 50 psia with air this is 50 x 0.0007029 = 0.0351 lb mole of air. With a molecular mass of 28.96 this gives 1.018 lb of air.
Now helium is added until the pressure is 100 psia so the TOTAL number of moles is
100 x 0.0007029 = 0.07029 lb mole. This means 0.0351 lb mole of helium has been added. With a molecular mass of 4 this is 0.1404 lb of helium.
At 200 psia there are 200 x 0.0007029 = 0.1406 lb mole of gas. Or 0.07029 lb mole of helium has been added, with a mass of 0.07029 x 4 = 0.2811 lb of helium.
The important, and non-intuitive, thing to note is that the pressure is proportional to number of moles of gas added, irrespective of the molecular mass of the gas (when the ideal gas law applies). In this example we see that much more air (in mass terms) must be added than helium to achieve the same pressure increase because helium has such a low molecular mass.
If your temperature is not 72 F you can easily rework the above with the right value.
Harvey