“…In these previous attempts at self-assembly, however, the nanoparticle superlattices obtained were usually highly symmetric structures, such as close-packed sixfold hexagonal lattices, fourfold cubic square lattices, and threefold quasi-honeycomb lattices. To enhance the versatility of nanoparticle superlattices, more complex and low symmetry ordered structures are also strongly desired, − especially in the case of magnetic materials, where it has been reported that the magnetic reversal and magneto-transport properties are strongly affected by the symmetry of the lattice arrangements, − and the presence of anisotropic periodic grooves or surface scratches can enhance the coercivity and remanent fields . For structural control of nanoparticle assembly, various procedures have been proposed, such as utilization of anisotropic nanoscale templates, ,, the application of external magnetic fields, − the tuning of interligand interactions, , the hybridization of multiple-sized nanoparticles, − and the utilization of nonspherical (cubic or rod-like) nanoparticles. − Nevertheless, to our knowledge, the spontaneous self-assembly of single-sized spherical nanoparticles into low-symmetry structures, such as twofold symmetric rectangular nanoparticle superlattices, with long-range periodic order has never been established.…”