The one thing I noticed about episode 5 in regards to Zemo: that man was ready to die.
This the face of a man that has lost his wife, his son and his country, everything but his money. He was ready to finally be with his family again like he wanted to be at the end of Civil War. Like it was said in the first episode, there is no word for a parent that's lost their child.
Now this is the face of a man disappointed that he won't be with his son and wife again, only to suffer more. He wanted Bucky to shoot him in the head, it'd hurt him less than continuing without those he's loved.