Maybe pick ones that can comment on your different abilities. For example, your PI can comment on research/lab skills. Others can comment on academic abilities, leadership skills, people skills, professionalism, etc.
Well, most schools like two science prof letter, and one non-science, plus one or two additional letters from doctors that you've shadowed, employers, research advisors, etc.
For the professor letters, ask ones that you've had multiple times and that you know fairly well. It is also good for your letters to be from senior members of the faculty, not TA's or associate professors (but those are okay in a pinch too for most schools).
You might also want to balance the letters. For example, one from a bio professor and another from a physics professor, as well as the non-science one.
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