When he knew he loved you:

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Thor: Thor wasn't used to being treated like a non-royal - No one was rude to him or ever told him what to do. That was until he met you, and you weren't afraid to tell him when he was being a stupid oaf. One day when you were snappy with him for something, he realised he loved you.  You treated him like a human, not a God or anyone higher, and it was just what he needed.

 Cap: He realised he loved you when he saw a definitive future with you. Everything in his life was uncertain and a bit messy, but you promised you would never leave and for once, he believed the words

 Banner: Bruce felt everyone was cautious around him. He realised he loved you when you trusted him and treated him like an actual human and not an unpredictable grenade.

 Stark: Tony realised he loved you when you didn't stop him doing stupid shit and actually started joining in. Bungee jumping off the Empire State? No problem. Throwing paint balls at a giant green rage monster? Excellent. He needed a literal partner in crime, and the fact you guys were an item made it all the better.

 Barton: Clint realised he loved you when he would take time out his job for you. He was metaphorically married to his job and it had become his life in every sense of the word. So when he didn't hesitate to take a day off to spend time with you, he realised you must be pretty damn important to him to.

Loki: He knew that almost nobody would ever trust him, he was a trickster after all. But, when you trusted him, it made him feel pretty damn special and I believe his exact words were ¨Petty humans giving me the so called 'feels.'¨

 Bucky: Bucky was a mess. He needed someone who he could confide in, someone who would be there. And once, you showed up at his house at 3 AM because he needed you. That was how he knew.

 fury : Nick never let anyone near his work, especially the most difficult work. But one day you asked to help and he willingly agreed, before realising what he had just done. He knew it must have been because he cared about you.

Coulson: He was showing you weapons one day and you two were messing around with things you probably shouldn't have. You laughed at one of his stupid jokes and he said your laugh was the best sound he'd ever heard. No matter how cliche it sounded.

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