If I had to pick a moment when Sasuke first began to fall in love with Sakura, I'd pick the moment when Sasuke stopped Sakura's fall after she used up nearly all her chakra to save his life.
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Sakura desperately gave everything she had to save Sasuke's life, a heroic act that wasn't overlooked by Sasuke. Rather than ignore that Sakura had just saved his life, Sasuke prevents her fall by teleporting by her side and gently catching her.
Sasuke closely studies her, as if seeing her in a new light and in a new way that he hadn't considered before. Her resolve to save him surprised him. Sasuke respects perseverance and hard work, and the extent of her efforts isn't lost on Sasuke. Previously Sasuke had largely overlooked Sakura as a warrior, but now she has gained his respect as a fighter. He'd assumed she would be of no help in the war, yet her determination and resolve have proven him wrong, as she had saved his life.
