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Train/bus between Florence, Montalcino and Rome?

We aren't renting a car, so we need to travel by train or bus. I tried to check http://www.trenitalia.com but it keeps telling me there is no solution so I assume there is no train.

Any ideas on how to travel, and/or pointers to web sites so I can check schedules?

Also, should I book these tickets in advance or should there be enough available seats to just buy them at the station when leaving? We're travelling by train Venice/Florence as well.

TIA - R.