CoovaChilli is the captive portal system, but you need something for it to authenticate against. This is usually a RADIUS server. In some circles this is known as a AAA server which stands for Authentication Authorisation and Accounting. The usual open source RADIUS server is FreeRADIUS which is excellent, but can be a bit daunting as there are so many options.
I've done it using YFi and CoovaChilli on PCs using Ubuntu. I have 13 Coova Chilli hotspots around the country being managed centrally from one YFi instance. But you can have both on one piece of hardware. I've never tried it on a Pi though.
It works very well on a PC. The YFi system is excellent, it allows you to set up vouchers, and permanent users. Even MAC address authentication and paid access. Walt the developer is very helpful. It uses MySQL and FreeRADIUS as a back end.
http://sourceforge.net/projects/hotcakes/
http://sourceforge.net/apps/trac/hotcak ... /WikiStart
http://www.coova.org/CoovaChilli