Hey Stefan,
You can configure your 5660 to start the acquisition by using a start trigger. One option would be to configure the trigger off of a digital edge on one of the PFI lines on the digitizer. Whenever a digital high is received on this line the acquisition would begin. Another option would be to send a software trigger. For example, if you pressed on a button on your VI you could configure it to send the software trigger and begin the acquisition.
As far as releasing the button and the acquisition stopping, this will be more difficult to implement. You could of course just a wire a stop button to your while loop to end the acquisition. If you need an actual hardware signal you could use a reference trigger. This will stop the acquisition after the reference trigger is received.
The driver ships with some example programs that should help you get started with this. If you look in the NI Example Finder in LabVIEW at Help » Find Examples » Hardware Input and Output » Modular Instruments » NI-RFSA (or NI-5660) » IQ Acquisition you should see an example called ni5660 Trigger IQ.vi. This will show you how this is implemented.
Good luck with your application and let me know if you have additional questions.
Regards,
Chris Delvizis
National Instruments