The first time I watched this episode, I thought Barnabas was an absolute idiot. He made it perfectly obvious to Angelique that he suspected something. This time around, I'm kinder. He had just suffered an enormous shock - greater than I can comprehend because I can't get into the "my wife" business. It would have been terrifically difficult for him not to betray any of his feelings. And maybe he was still hoping that Angelique would somehow prove that she was not a witch. Still, sitting and staring at the portrait of Josette was distinctly ill-advised. Barnabas knows what Angelique has done in the past, but he seems to be incapable of thinking about what Angelique might do in the future.
What does Angelique think love is? I can't imagine believing I was in love with someone if I had to keep a huge part of my life secret from him - but that's what Angelique is doing. She lies to him every minute of the day, it seems - although of course we don't see every minute, and in particular we don't see much of the minutes in which she isn't lying, because they aren't so interesting or satisfying to the audience. I suppose her idea is that once they get away from Collinsport, she'll be able to leave the witchcraft behind as well. If that's the case, then once again she's deceiving herself. Witchcraft will always be her first resort.