Putting the keywords in the title twice isn't going to help any more than once and could get you penalized for KW stuffing. I would avoid putting the keywords in there twice. Also there is no set rule about a 66 character limit in the title. I suggest that having less characters in the title with the targeted search terms in there only once will give more weight to the keywords without the possibility of any penalties for keyword stuffing.
It is only my opinion of course but the keywords don't appear anywhere near enough times to be penalized for keyword stuffing. I actually think including the term twice in relation to the rest of the text gives quite a nice keyword density from experience. I suppose it's a question of whether to include the initial keyphrase at the start of the title. I think in this situation it add's more weight to the keyphrase and includes the additional relevency benefit of having the keyphrase at the very start of the title tag.
I have seen debates on placing the keywords at the front to get more weight and from my personal experience, I don't think it really adds that much more weight if any. I don't think that having the keywords 2 words into the title will have any more weight that having it at the front. Now if the title was really long then yes, you would want the keywords right at the front rather than 10 or 12 words into the title.