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Split -> Zagreb -> Ljubljana -> Zagreb

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Hi everyone,
I'm visiting Croatia and Slovenia in a few days and need some help planning my transport.
I fly into Split and leave from Zagreb. My plan is to take the bus from Split to Zagreb, then visit some friends in Ljubljana (by train) for a couple of days before returning to Zagreb for my outbound flight. Just a couple of questions --

1) Is it necessary to buy the Split-Zagreb bus tickets in advance? If so, how far ahead?
2) Is train the best way to travel between Zagreb and Ljubljana? And again, how far ahead should I buy the tickets?

Thank you for your help!

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