Deterministic assembly of single emitters in sub-5 nanometer optical cavity formed by gold nanorod dimers on three-dimensional DNA origami

被引:0
作者
Zhi Zhao
Xiahui Chen
Jiawei Zuo
Ali Basiri
Shinhyuk Choi
Yu Yao
Yan Liu
Chao Wang
机构
[1] Arizona State University,Center for Molecular Design and Biomimetics at the Biodesign Institute
[2] Arizona State University,School of Molecular Sciences
[3] Arizona State University,School of Electrical, Computer and Energy Engineering
[4] Beijing University of Technology,Faculty of Materials and Manufacturing, Key Laboratory of Advanced Functional Materials, Education Ministry of China
来源
Nano Research | 2022年 / 15卷
关键词
DNA origami; self-assembly; deterministic single emitter; plasmonic nanocavity; nanorod dimer; optical coupling;
D O I
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中图分类号
学科分类号
摘要
Controllable strong interactions between a nanocavity and a single emitter is important to manipulating optical emission in a nanophotonic system but challenging to achieve. Herein a three-dimensional DNA origami, named as DNA rack (DR) is proposed and demonstrated to deterministically and precisely assemble single emitters within ultra-small plasmonic nanocavities formed by closely coupled gold nanorods (AuNRs). Uniquely, the DR is in a saddle shape, with two tubular grooves that geometrically allow a snug fit and linearly align two AuNRs with a bending angle < 10°. It also includes a spacer at the saddle point to maintain the gap between AuNRs as small as 2–3 nm, forming a nanocavity estimated to be 20 nm3 and an experimentally measured Q factor of 7.3. A DNA docking strand is designed at the spacer to position a single fluorescent emitter at nanometer accuracy within the cavity. Using Cy5 as a model emitter, a ∼ 30-fold fluorescence enhancement and a significantly reduced emission lifetime (from 1.6 ns to 670 ps) were experimentally verified, confirming significant emitter-cavity interactions. This DR-templated assembly method is capable of fitting AuNRs of variable length-to-width aspect ratios to form anisotropic nanocavities and deterministically incorporate different single emitters, thus enabling flexible design of both cavity resonance and emission wavelengths to tailor light-matter interactions at nanometer scale.
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页码:1327 / 1337
页数:10
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