It could be he was thinking aout Haldir, or that he realised that (for him at least) the war was not over and that there would be many more deaths. We'll have to wait until Jackson explains in the commentary on the EE I suppose.
Other bits I've noticed:
How much gollum looks like Andy Serkis just before they go into Shelob's tunnel. It is stunning.
How Jackson has taken the pictures Alan Lee for the centenary edition of the LOTR book, and used in the movie. The steps leading up to Cirith Ungol where Frodo's attacked by Shelob is one. (Helm's Deep wall being another).
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