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In my view it's when Shinji's using (or trying to use) his own initiative, rather then doing what others want. The 'twich' is when hes thinking about or trying to do this, and then the clench is when hes succeeded and hes going all out. It's about him gaining confidence and getting what he wants. The scene where the kids laugh at him always struck me as deep and sad one. Shinji's just starting to feel confident, partly due to him just becoming the top sync ratio holder. Shinji clenching his fist on the bus when theres no situation for it shows that he's feeling confident in every day life. Thinking 'I can do this', but then hes laughed at for it, and it's kids laughing at him no less. Very degrading. What's worse is later on in that episode, after a second clench and show of confidence, he's f'd up by an Angel because of it. It's poor old Shinji constantly gaining confidence, being assertive, and then having the rug swept from under his feet because of it. Fueling his 'do what others tell you or do nothing' attitude to life.
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