As an analyst, I've tried multiple approaches:
- just e-mail
- Excel spreadsheets
- specialized sw such as Enterprise Architect
I found out that in order to bring all the people to the table (it being the SAME table is a critical concern), you've got to have a system that is accessible to the business people (who own the requirements) and also by the development team.
And so when you want to have really good requirements, clarified beyond any doubt and agreed upon by everybody, it pays to have a system that the business people will use. No experience with LucidSpec; concerning GUI mockups, I have found from my own recent experience that non-imposing, playful apps such as Balsamiq can "draw" the business people into the game and get them think about what they want - great for gathering and analyzing requirements.
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[SELF-PROMO] You could test-drive Playground, a web app for writing requirements and specs that my company is operating. It's on the casual side and encourages cooperation between the owner / analyst and the development team.