biostudies-literatureKim JYDOD | USN | Office of Naval Research (ONR)Center of Complex Particle Systems (COMPASS)DOD | USN | Office of Naval ResearchNational Science Foundation (NSF)DOD | USAF | AMC | Air Force Office of Scientific ResearchCenter of Complex Particle SystemsDOD | USAF | AMC | Air Force Office of Scientific Research (AFOSR)National Science Foundatione2312082121https://www.ebi.ac.uk/biostudies/studies/S-EPMC10945859biostudies-literatureUnknown121(11)Chiral plasmonic surfaces with 3D "forests" from nanohelicoids should provide strong optical rotation due to alignment of helical axis with propagation vector of photons. However, such three-dimensional nanostructures also demand multi-step nanofabrication, which is incompatible with many substrates. Large-scale photonic patterns on polymeric and flexible substrates remain unattainable. Here, we demonstrate the substrate-tolerant direct-write printing and patterning of silver nanohelicoids with out-of-plane 3D orientation using circularly polarized light. Centimeter-scale chiral plasmonic surfaces can be produced within minutes using inexpensive medium-power lasers. The growth of nanohelicoids is driven by the symmetry-broken site-selective deposition and self-assembly of the silver nanoparticles (NPs). The ellipticity and wavelength of the incident photons control the local handedness and size of the printed nanohelicoids, which enables on-the-fly modulation of nanohelicoid chirality during direct writing and simple pathways to complex multifunctional metasurfaces. Processing simplicity, high polarization rotation, and fine spatial resolution of the light-driven printing of stand-up helicoids provide a rapid pathway to chiral plasmonic surfaces, accelerating the development of chiral photonics for health and information technologies.Proceedings of the National Academy of Sciences of the United States of AmericaDirect-write 3D printing of plasmonic nanohelicoids by circularly polarized light.PMC10945859CHE-1807676HQ00342010033FA9550-20-1-0265NSF 2243104.ONR N000141812876N00014-20-1-2479Pfaffenberger ZJKim STurali Emre ESChoi WKim JYBiteen JSCha MMcGlothin CKotov NAfalseDirect-write 3D printing of plasmonic nanohelicoids by circularly polarized light.Chiral plasmonic surfaces with 3D "forests" from nanohelicoids should provide strong optical rotation due to alignment of helical axis with propagation vector of photons. However, such three-dimensional nanostructures also demand multi-step nanofabrication, which is incompatible with many substrates. Large-scale photonic patterns on polymeric and flexible substrates remain unattainable. Here, we demonstrate the substrate-tolerant direct-write printing and patterning of silver nanohelicoids with out-of-plane 3D orientation using circularly polarized light. Centimeter-scale chiral plasmonic surfaces can be produced within minutes using inexpensive medium-power lasers. The growth of nanohelicoids is driven by the symmetry-broken site-selective deposition and self-assembly of the silver nanoparticles (NPs). The ellipticity and wavelength of the incident photons control the local handedness and size of the printed nanohelicoids, which enables on-the-fly modulation of nanohelicoid chirality during direct writing and simple pathways to complex multifunctional metasurfaces. Processing simplicity, high polarization rotation, and fine spatial resolution of the light-driven printing of stand-up helicoids provide a rapid pathway to chiral plasmonic surfaces, accelerating the development of chiral photonics for health and information technologies.2024-01-01T00:00:00Z2024 Mar2026-06-29T03:18:59.675Z2025-05-18T12:54:27.533ZS-EPMC109458593844685410.1073/pnas.2312082121