Moonsols is a great option, but I've noticed that there is no longer an option to purchase it and it makes me wonder if support has been stopped.
In my opinion, the best way to get started is with win32dd, win64dd, or mdd. Another option that is more automated is DumpIt (created by the maker of Moonsols). I prefer mdd for most tasks, but I have not tested it on 64bit systems.
Depending on what you're looking for, I tend to use file carvers like Scalpel to pick out everything that is recognizable. Volatility is nice too, but personally I think learning how to recognize the file structures in a hex editor and carving them out will lead you to a better understanding of the dumped memory and what you're actually looking at.
The newest version of scalpel is available in Backtrack r3, I just pulled it from there. As with the others, I have older copies that I use and they work just fine. DumpIt is still available at the MoonSols site and works great for 32 or 64bit, give it a shot: moonsols.com/2011/07/18/moonsols-dumpit-goes-mainstream