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The heaviest nuclei where excitations above the ground state can be studied lie near Z ~ 100. These nuclear structure studies are important testing grounds for theoretical models that aim to describe superheavy nuclei. To study the highest neutron orbitals (150 ≤ N ≤ 154), we have populated high angular momentum states in a series of Pu (Z = 94), Cm (Z = 96) and Cf (Z = 98) nuclei, via inelastic and transfer reactions, with heavy beams on long-lived radioactive actinide targets. Multiple collective excitation modes and structures were identified, and their configurations deduced. Quasiparticle alignments are mapped, with odd-A band structures helping identify specific orbital contributions via blocking arguments. Higher-order multipole shapes are observed to play a significant role in disentangling competing neutron and proton alignments. The N > 152 data provide new perspectives on physics beyond the N = 152 sub-shell gap.