Another way of looking at it: You can write whatever you want on paper and sign it, but that doesn't make it enforceable. You could sign a document that makes you a slave or puts up your children as collateral for your ISP bill, but those agreements would be scrap paper (or evidence for the prosecutor).
(a) They are regarded as seeking admission and they are found inadmissible. Refusing to unlock their device will not make an LPR regarded as seeking admission as it’s not a reason listed in INA 101 (a)(13)(C): https://www.uscis.gov/ilink/docView/SLB/HTML/SLB/0-0-0-1/0-0...
(b) They are deportable. Simply refusing to unlock a device in itself will not make someone deportable as it’s not listed in INA 237 “General Classes of Deportable Aliens”: https://www.uscis.gov/ilink/docView/SLB/HTML/SLB/0-0-0-1/0-0...
Since I work for an educational institution, there is potentially FERPA protected data on my drive. In some instance we also deal with HIPPA data. It's also interesting because my password manager stores it's data as encrypted files on that drive (mirrored from the cloud). I'm certainly not unlocking that either.