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For Amazon Music Unlimited tracks, is it possible to switch between Dolby Atmos and Ultra HD within the S2 app (presuming both formats are available for the track being played)?

You can switch easily enough in the Amazon app.

If you disable the “Spatial Music” setting in room settings it should switch to HD/UHD for the current track. However IIRC re-enabling “Spatial Music” will only take effect when the next Atmos track starts.