Purely in terms of melody, I really like Eowyn's lament in Rohan - it's simple, and evocative in itself but doubly powerful when coupled with her acting.
I thought Pippin's song in Minas Tirith is a good example of how a musical piece can really have a profound effect on the audience with some strategic editing. I don't particularly love the tune, but it's very fitting for the scene.
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Caelum videre iussit et erectos ad sidera tollere vultus.
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