DR NO's casino scene almost occupies a parallel universe in what it represents, and how well it introduces the character.
Looking beyond that, you could pretty much make a convincing case for any of the others. Despite other obvious inconsistencies through the series, the casino scenes are fairly strong as a rule.
My favourites: SKYFALL is incredibly atmospheric; THUNDERBALL has a tremendously tense face-off; GOLDENEYE reminded everybody who and what Bond was after a six-year hiatus.