摘要： An economically scalable and reproducible method to assemble nanoparticles (NPs) into ordered arrays with high fidelity remains a fundamental roadblock. Methods like directed self-assembly have shown the highest promise resulting in >85% density of NP-filled prepatterned polymer cavities. This work refines directed self-assembly by controlling the evaporation rate, substrate velocity (deposition rate), and NP diameter resulting in reproducible fabrication of ordered arrays with areas >2 mm × 2 mm and ~100% density of filled cavities. Measured optical spectra showed a blueshift in the localized surface plasmon resonance (LSPR) and surface lattice resonance (SLR) peaks with increasing NP density for both 100 and 150 nm gold (Au) NPs. Discrete dipole approximation (DDA), coupled dipole approximation (CDA), rapid semi-analytical CDA (rsa-CDA), and Mie theory simulations closely matched extinction per nanoparticle (extinction/NP) calculations for measured extinction spectra. An ordered array containing 150 nm AuNPs was used for comparison with rsa-CDA estimates using both polydimethylsiloxane (PDMS) and glass refractive indices (RI) resulting in peak location estimates within 1.7% and comparable relative increases in peak heights. Both the measured and simulated SLR peak heights were shown to significantly increase when the array was on glass as opposed to within PDMS.