Are there any (preferably free) tools which would let you throw together a quick outline of a UI, and build these into storyboards to create a mockup of how a use-case might play out including popup dialogs that could be raised, etc?
Not really a storyboard, but Mockingbird allows you to create multiple pages.
If you have Microsoft PowerPoint, Apple Keynote or OpenOffice you can use that as well. Such applications work really good for mockups, and they show a list of slides ( storyboard-items =D ).
Good luck.
Maybe you will be interested in ForeUI, which creates working prototype with flowchart instead of storyboard.
From my experience I have seen a lot of UI Designers use PowerPoint given it's flexibility and natural abilities to present the UI design to stakeholders.
Here is a good article on the benefits of using PowerPoint posted on UX-Magazine.
http://uxmag.com/articles/wireframing-in-powerpoint-it-works
This will provide you with a capable free UI mockup tool that is not limited to the ui controls pallet found in most wireframe mockup tools.
For a very small amount of money you should consider purchasing PowerMockups (http://www.powermockups.com) which provides a pallet of already defined UI Controls, that is extensible with your own creations. I have used this tool and found it to save time building common UI Controls, and also when I want to craft a unique UI Control I can add it to the pallet and re-use it on other UI Mockups.
There is also a product called PowerStory http://www.power-story.com which will allow you to take your UI Mockups and build a UI Storyboard in PowerPoint that supports the ability to define main flows and alternate flows as you would see in use cases. It will also generate test cases into TFS from your UI Mockups.
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