Self-Organized Phase-Composite Nanocrystal Solids with Superior Charge Transport

Interparticle electronic coupling is essential for self-assembled colloidal nanocrystal (NC) solid semiconductors to fulfill their wide-tunable electrical and optoelectrical properties, but it has been limited by disorders. Here, a disorder-tolerant coupling approach is presented by synthesizing self-organized NC solids based on amorphous/nanocrystalline phase-composites. The ZnO amorphous matrix, which infills the space between the less regularly ordered ZnO NCs, enables robust electronic coupling between neighboring NCs via the resonant wave function overlap, leading to a disorder-tolerant resonant conducting state. Field-effect transistors based on phase-composite semiconductors show delocalized band-like transport with superior field-effect mobility values (∼75 cm² V^-1 s^-1), compared to amorphous or polycrystalline ZnO semiconductors. Furthermore, the broad amorphous matrix can mitigate interfacial defects between crystalline regions through atomic relaxation, in contrast to narrow grain boundaries in polycrystalline films, resulting in a significantly low interface trap density for phase-composite NC solids. Density function theory calculations and quantum transport simulations using the nonequilibrium Green's function formalism elucidate the origins of superior and highly disorder-tolerant electron transport in phase-composite NC solids. Our report introduces a new class of NC solids complementary to the colloidal counterpart and will be applicable to CMOS-compatible emerging device technologies.