Bucky mentally preparing himself for death is so fucking upsetting because after all of the torture he went through, after all of the physical and mental pain, he survived because Steve saved him, and here he is ready to die for him. He lets himself have this moment of fear because he knows what’s coming, he knows that he’s going to die and he allows himself to accept how scared he really is. He knew what he was getting in to when he made the choice to fight side by side with Steve (because what other choice was there really?), and part of him probably always knew this was how it would end - he was either going to live for Steve or die for him, the only thing left for him to do was to acknowledge his unhappy ending when the time came.
(FRIENDLY REMINDER THAT POSITIONING BUCKY’S SACRIFICE AS HIS CHOICE MEANS THAT IT WAS THE LAST TIME HE EVER GOT TO EXERCISE HIS OWN FREE WILL.)
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His “resurrection” as the Winter Soldier is a denial of his right to die, his right to decide what to do with his life, his body. That type of control is a horror that we tend to think of as a horror above or beyond death; there is something worse than death, and it is losing what we think of as the basic embodied human right of inhabitation of, autonomy over one’s own body. That’s what he’s about to suffer, and it kind of turns this scene from tragedy into horror