Have said this before, but THE single best sequence of the series, is the long tracking sot during Spock's breakdown in The Naked Time. Not only is beautifully written and acted, but Daniels and Finnerman NAILED it in ONE take - while the clock was ticking on the shooting schedule for the day!
There are a few other shots/sequences that Daniels and Finnerman also absolutely hit the bullseye on, that still reasonate emotionally to this day:
The entire last five minutes of The Menagerie after the viewer shuts off. Shatner and Nimoy have never been better, and when Spock wheels Pike out of the BR, after telling Kirk 'I believe I have handled this whole matter in a totally logical manner", THEN he lowers his head in a somber manner....it just gets ya right in the heart. And then, when the Keeper shows Kirk the rejuvenated Pike, after all the crap KIRK had been through, Kirk is able to show a smile for his old friends happiness, that too, is an amazing piece of acting and direction.
The business in MM where the MU Sulu tries to bully Spock about his orders to kill Kirk, and Spock totally sees through his 'threat', and basically tells him, "Don't fuck with me boy, I have Vulcans working for me!" - Sulu's reaction is PRICELESS....
When in DM, Decker trying to describe the planet killer, and then when Decker is in the shuttle, preparing himself for his doom,,amazing stuff!