The best way right now to buy steam games is to do it from your web browser. You can use your regular web browser, it does not have to be within the crossover environment.
Go to http://store.steampowered.com/
Search for the game(s) you would like to purchase.
Click add to Cart
If you wish to continue shopping choose continue shopping, and repeat the above steps. Otherwise click purchase for myself.
You will be prompted to log in, do so.
You will be prompted to accept the steam agreement, if you accept the terms, proceed.
Enter your payment information, and from there it should be pretty straight forward.
The game will be added to your Steam games list once the transaction is completed. The game will automatically be ready to start downloading when you open steam.
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