Personally I found even one child in a high position, ie the rear seat, was less stable than I’d like when getting us both mounted and dismounted (ie it’s far too easy for the bike to topple); no way would I try two, but YMMV. Maybe with a very solid twin-leg kickstand, I suppose, but not without.
The safer options are, I’d have thought: a trailer (probably impossible on the train), a bakfiets or similar (very expensive, and probably still a nightmare on the train), a Follow-Me tandem (assuming you’re dropping the 4yo off first and can store their bike there, then you can fold up the Follow-Me on your own bike, or find a route where the 4yo can ride themselves.
You can get cheap trailers, eg the Halfords ones, which can be detached and folded flat (wheels off, too) in about a minute… maybe easier to store at nursery than a tagalong?