Hard to say, considering I only have the second two.
I have a soft spot for the minor key, so I'd go with "the Uruk-hai" as a nice little evil ditty to hum. I always though Howard Shore was great at characterizing the races and peoples into music. I thought that the classical beat with that oh-so-lovely metallic drumming in the background was just perfect for Isengard, and the celtic melancholiness of the fiddle great for Rohan.
Overall, I liked "The Uruk-hai", "The White Tree", "The Return of the King", and "Into the West"
By the way, to add a side note, the stunning Rohan theme is actually played by a single Norwegian Fiddle. I had the great luck to obtain the music (being a violinist myself) and am rather adept at it if I do say so myself. (shameless self-promotion).
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"What mortal feels not awe/Nor trembles at our name,
Hearing our fate-appointed power sublime/Fixed by the eternal law.
For old our office, and our fame,"
-Aeschylus, Song of the Furies
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