Unless The Chief has a way to shield his tech from techno-paths he is going to seriously struggle here.
Smarter is kinda a loaded question, Pym is considered a leading expert in multiple scientific areas from Robotics to Physics to Med to Biology. He's probably also outside of Doom the only "Top Ten" guy to use magic in his inventions. (Granted he can't produce magic)
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I think the Chief might be more versatile in science. Here are some feats, taken from Desaad:
-The Chief has invented a time machine
- replaced the JLA's abilities with tech approximations.
-Brought Rita back from the dead with just a piece of her skull.
-created nanobots that could literally do anything, including create a being so powerful that he was throwing his victims through the fourth wall into 'our' reality.
-And it looks like he's going to discover away to alter his genes so that he becomes Kryptonian. (Which he successfully did).
Pym has 2 time machines (one normal, one built around Nico's magic)
Pym built Ultron who alone gives the avengers solid fights, and since the fusion he/it is comfortably in the Trans tier being casually more powerful than the combined might avengers.
Pym reassembled Korvac's wife from scattered atoms, though he did at first think it was Janet.
Ultron's "son" at the conclusion of Avengers AI killed Galactus and forced his way into the realm of God. (depicted as Allah)((as a bald parrot))
That last one is outside Pym's specialty, but Ultron has a techno-virus that turned a planet into a ship for him, and converts living beings into Ultron shells.
The range of Caulder's knowledge is vast.
In the last DP run he was the go to guy for scentists of every field.
I didn't like the change in that run that made him a manipulative bastard who basically manipulated the members of the DP into having their powers and actually causing their accidents.
Having said that Caulder was basically showing only real world science and meta gene stuff, and Pym is one of the very few scientists who has also cracked the nature of magical energy and been able to use science to affect it ( Micheal Holt and Lex Luthor , the only other ones that comes to mind, and Lex was dismally defeated on it by Vic Sage Question).
Caulder is certainly up there where DCU earth brains are concerned but I'd have to give a slight nod to Pym all things considered.
I mean seriously General Immortus got the better of Caulder a few to many times.
Which run are you referring to? Certainly not Giffen's run. He was bringing people back from the dead and giving himself Kryptonian powers. Among other crazy shit.