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Deterministic assembly of single optical cavity formed by gold dimensional DNA origami

查看全文 作  者:Zhi [1,3,4]Zhao;Xiahui [3]Chen;Jiawei [3]Zuo;Ali [3]Basiri;Shinhyuk [3]Choi;Yu [3]Yao;Yan [1,2]Liu;Chao [1,3]Wang 高影响力作者 机构地区:[1]Center for Molecular Design and Biomimetics at the Biodesign Institute,Arizona State University,Tempe,Arizona 85287,USA;[2]School of Molecular Sciences,Arizona State University,Tempe,AZ 85287,USA;[3]School of Electrical,Computer and Energy Engineering,Arizona State University,Tempe,AZ 85287,USA;[4]Faculty of Materials and Manufacturing,Key Laboratory of Advanced Functional Materials,Education Ministry of China,Beijing University of Technology,Beijing 100124,China高影响力机构 出  处:《Nano Research》索引2022年第15卷第2期,共11页高影响力期刊 基  金:support from an Army Research Office MURI award no.W91 INF-12-1-0420;C.W.thanks the ASU startup funds and National Science Foundation under grant Nos.1711412,1838443,and 1847324 for partially supporting this research;Y.Y.thanks the ASU startup funds and National Science Foundation under grant Nos.1809997 for partially supporting this research. 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 nm^(3) and an experimentally measured O 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. 关 键 词:DNA origami self-assembly deterministic single emitter plasmonic nanocavity nanorod dimer optical coupling
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