You probably meant here “which elements are the largest atoms”, meaning which elements have the largest atomic radius. The elements with the largest atomic radii are located towards the left and bottom of the periodic table (i.e. At the bottom of Group 1). Thus, in theory, the largest atom should be Francium. Researchers operating the world's largest and most powerful particle accelerator may be closer to discovering the secrets of our universe, because it has rec. World's Largest Atom Smasher Breaks Record Scientists are celebrating after the Large Hadron Collider started making atomic particles head-on at record-breaking energies. The $10 billion.
If by 'biggest' and 'smallest', you mean mass (which is a measure of how much matter is there), then the smallest is the hydrogen atom with one proton and one electron. Since electrons are about 2000 times less massive than protons (and neutrons), then the mass of an atom is mostly from the protons and neutrons.
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Or watch our full Atoms game webinar here.