You can see they're attracted to each other the second they meet. I really doubt the Captain spent the same amount of time talking to the previous governesses that he spends talking to Maria. It would be how do you do, and then the housekeeper would probably tell Maria the rest.
In the movie, the captain sounds stern, but he's eyeing up Maria a lot, tells her she looks nothing like a governess, and is always checking to see how she's reacting to what he says. When she's cheeky with him it leaves a mark. If this were a regular, standard-issue governess he wouldn't have stuck around in the entrance hall as long as he did, or paid much attention to what she said or how she said it.
I actually see his attraction to her more immediately than hers to him, although she is playful with him - especially her facial expression. But she's certainly not intimidated by him. He's an impatient guy with a lot of stuff on his mind - if she didn't interest him he wouldn't be in tune with what she said, did and thought, and he is from the start. In the entrance hall, and then at the dinner table.
I think when he returns from Vienna with the Baroness, he's curious to see Maria again. I also think when he's angry, it's way OTT and maybe an excuse to get rid of her so she'll stop distracting him. But then he realizes she brings something needed into the house.
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