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Title: 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. Finally, this approach providesmore » the basis for rational creation of single-emitter 3D nanodevices with controllable polarization output using a highly customizable DNA assembly platform.« less

Authors:
ORCiD logo [1];  [1];  [2];  [1]; ORCiD logo [1];  [3];  [3]; ORCiD logo [1]; ORCiD logo [1];  [4]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Xi'an Jiatong Univ. (China)
  3. Northrop Grumman Corporation, Redondo Beach, CA (United States)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Columbia Univ., New York, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1607973
Report Number(s):
BNL-213780-2020-JAAM
Journal ID: ISSN 1936-0851
Grant/Contract Number:  
SC0012704; SC0008772
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 14; Journal Issue: 2; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; quantum dots; nanoparticle cluster; fluorescence; polarization; self-assembly; DNA nanotechnology

Citation Formats

Zhang, Honghu, Li, Mingxing, Wang, Kaiwei, Tian, Ye, Chen, Jia-Shiang, Fountaine, Katherine T., DiMarzio, Donald, Liu, Mingzhao, Cotlet, Mircea, and Gang, Oleg. Polarized Single-Particle Quantum Dot Emitters through Programmable Cluster Assembly. United States: N. p., 2019. Web. https://doi.org/10.1021/acsnano.9b06919.
Zhang, Honghu, Li, Mingxing, Wang, Kaiwei, Tian, Ye, Chen, Jia-Shiang, Fountaine, Katherine T., DiMarzio, Donald, Liu, Mingzhao, Cotlet, Mircea, & Gang, Oleg. Polarized Single-Particle Quantum Dot Emitters through Programmable Cluster Assembly. United States. https://doi.org/10.1021/acsnano.9b06919
Zhang, Honghu, Li, Mingxing, Wang, Kaiwei, Tian, Ye, Chen, Jia-Shiang, Fountaine, Katherine T., DiMarzio, Donald, Liu, Mingzhao, Cotlet, Mircea, and Gang, Oleg. Thu . "Polarized Single-Particle Quantum Dot Emitters through Programmable Cluster Assembly". United States. https://doi.org/10.1021/acsnano.9b06919. https://www.osti.gov/servlets/purl/1607973.
@article{osti_1607973,
title = {Polarized Single-Particle Quantum Dot Emitters through Programmable Cluster Assembly},
author = {Zhang, Honghu and Li, Mingxing and Wang, Kaiwei and Tian, Ye and Chen, Jia-Shiang and Fountaine, Katherine T. and DiMarzio, Donald and Liu, Mingzhao and Cotlet, Mircea and Gang, Oleg},
abstractNote = {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. Finally, this approach provides the basis for rational creation of single-emitter 3D nanodevices with controllable polarization output using a highly customizable DNA assembly platform.},
doi = {10.1021/acsnano.9b06919},
journal = {ACS Nano},
number = 2,
volume = 14,
place = {United States},
year = {2019},
month = {12}
}

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