colloidal crystals (CCs) constructed from inor-ganic nanoparticle (NP) building blocks exhibit properties thatcannot be realized from isolated NPs or corresponding bulkcounterparts. Because the arrangement of NPs in CCs is crucial inthe CC's collective properties, development of a procedure tomodulate the assembly of NP constituents is important. Wedemonstrate rapid formation of nickel (phosphide) CCs withtunable crystallinity through van der Waals force-driven sponta-neous self-assembly of NPs in a facile one-pot colloidal synthesis.The quantity of size-regulating reagent (tri-n-octylphosphine)modulates the assembly of NPs from ordered close-packed to adisordered configuration in CCs. Synchrotron-basedin situsmall-angle X-ray scattering revealed that the size uniformity of the NPsdetermines the crystallinity of CCs, indicating the importance of regulating the growth kinetics of NPs during the synthesis. Ourwork will be useful for universal scalable preparation of CCs from a variety of materials and structures, with tunable concertedproperties.
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