I quite like their last one - Le Voyage Dans La Lune, though it must be said I also like Georges Melies for whose 1912 film this is the soundtrack. Combines the best elements of a soundtrack for a silent movie -using music to convey emotions or atmospheres - with the trip-hopish elements of their earlier work.
As an accompaniment to a silent movie, probably only Cinematic Orchestra's Man with a Movie camera comes close. Moroder's Metropolis was an abomination and Glass' Nosferatu nowhere near scary enough.
regards,
Giles