(Polar molecules, Non-polar molecules, etc.)
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VESPR determines the shape of a molecule based on the number of electron pairs surrounding the central atom. MOT is also a way to determine molecular structure, but the electrons are not stuck in one bond, rather, they are spread out throughout the entire molecule. This is a more accurate representation of the electrons in a molecule.
VSEPR is a way for one to determine the shape and the way that certain atoms bond to each other and their angles. MOT is a way to describe the valence electrons of those atoms who are bonded to each other.
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