Far more likely he'll approve airstrikes using the MOP bunker-buster in an attempt to take out the underground enrichment facilities the Israelis don't have the ordnance to deal with. I imagine there are plenty of other targets he'll approve for airstrikes, perhaps including Khamenei himself, always assuming we can find him now since Trump blurted out that we knew where he was and were just choosing not to strike.
Dropping bunker-busters on their labs or blowing up other infrastructure is one thing. Assassinating Khamenei, though, is far and away something else and would be a very dangerous escalation on the entire world stage. Most nations have a sort of unspoken "gentlemen's agreement" that they won't try to assassinate the heads of state of other nations. Crossing that line would be a big deal.
In any case, I'll be extremely shocked if Trump authorizes boots on the ground in Iran beyond using special forces in select roles. It's one thing to blow their shit up from the air, quite another to send in thousands and thousands of troops.