Polarized Single-Particle Quantum Dot Emitters through Programmable Cluster Assembly

Abstract

Although fluorescence and lifetimes of nanoscale emitters can be manipulated by plasmonic materials, it is harder to control polarization due to strict requirements on emitter environments. An ability to engineer 3D nanoarchitectures with nanoscale precision is needed for controlled polarization of nanoscale emitters. Here, we show that prescribed 3D heterocluster architectures with polarized emission can be successfully assembled from nanoscale fluorescent emitters and metallic nanoparticles using DNA-based self-assembly methods. An octahedral DNA origami frame serves as a programmable scaffold for heterogeneous nanoparticle assembly into prescribed clusters. Internal space and external connections of the frames are programmed to coordinate spherical quantum dots (QDs) and gold nanoparticles (AuNPs) into heterocluster architectures through site-specific DNA encodings. We demonstrate and characterize assembly of these architectures using in situ and ex situ structural methods. These cluster nanodevices exhibit polarized light emission with a plasmon-induced dipole along the QD-AuNP nanocluster axis, as observed by single-cluster optical probing. Moreover, emittance properties can be tuned via cluster design. Through a systematic study, we analyzed and established the correlation between cluster architecture, cluster orientation, and polarized emission at a single-emitter level. Excellent correspondence between the optical behavior of these clusters and theoretical predictions was observed. This approach provides the basis for rational creation of single-emitter 3D nanodevices with controllable polarization output using a highly customizable DNA assembly platform.