I've watched this thread while out of town, and been thinking how you might 'linearize' the testing, which dates to something CAR and DRIVER talked about back in 1978.
If you had access to a constant-grade portion of some mountain highway, say 3%, and there was some slack time where traffic would permit it, a fully-warmed vehicle, in neutral, would reach a 'terminal velocity' signifying a force equal to 3% of the mass of the vehicle.
This velocity would just compensate for aero and R-R.
Knowing the original Cd and frontal area would allow one to calculate the rolling force coefficient for the tires.
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If the terminal velocity increased after drag were reduced, while holding vehicle weight constant, the new R-R portion could be calculated for the higher speed, and factored in to isolate the only Cd which could explain the speed increase.
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It would get rid of all the differential calculus required to solve for two unknowns simultaneously.
Gravitational constants don't change.
Air density wouldn't change appreciably, if the aero mods could be added/subtracted in a short time period.
The car would still be 'warmed up', so non- thermally-equilibrated testing wouldn't rear it's ugly head.
Wind might not change appreciably in a short time domain.
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I drove from Pest-Buda, north, into Slovakia and the Taurus Mountains once. I wasn't thinking about it then, but there might have been places which might have lent themselves to testing like this.
Austria, Slovenia, Romania, Serbia, etc., all might offer opportunities.
Just a thought.
Coastdowns remain a daunting task. One year, there were only eleven days where the weather was good enough to do any outdoor testing in all of England.
It's why we have wind tunnels and CFD.