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Title: Dynamically controlled Purcell enhancement of visible spontaneous emission in a gated plasmonic heterostructure

Abstract

Emission control of colloidal quantum dots (QDs) is a cornerstone of modern high-quality lighting and display technologies. Dynamic emission control of colloidal QDs in an optoelectronic device is usually achieved by changing the optical pump intensity or injection current density. Here we propose and demonstrate a distinctly different mechanism for the temporal modulation of QD emission intensity at constant optical pumping rate. Our mechanism is based on the electrically controlled modulation of the local density of optical states (LDOS) at the position of the QDs, resulting in the modulation of the QD spontaneous emission rate, far-field emission intensity, and quantum yield. We manipulate the LDOS via field effect-induced optical permittivity modulation of an ultrathin titanium nitride (TiN) film, which is incorporated in a gated TiN/SiO2/Ag plasmonic heterostructure. In conclusion, the demonstrated electrical control of the colloidal QD emission provides a new approach for modulating intensity of light in displays and other optoelectronics.

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [2];  [2];  [2];  [2];  [2];  [2]
  1. California Inst. of Technology (CalTech), Pasadena, CA (United States); Academia Sinica, Taipei (Taiwan)
  2. California Inst. of Technology (CalTech), Pasadena, CA (United States)
Publication Date:
Research Org.:
California Institute of Technology (CalTech), Pasadena, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1499680
Grant/Contract Number:  
FG02-07ER46405
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING

Citation Formats

Lu, Yu -Jung, Sokhoyan, Ruzan, Cheng, Wen -Hui, Shirmanesh, Ghazaleh Kafaie, Davoyan, Artur R., Pala, Ragip A., Thyagarajan, Krishnan, and Atwater, Harry A. Dynamically controlled Purcell enhancement of visible spontaneous emission in a gated plasmonic heterostructure. United States: N. p., 2017. Web. doi:10.1038/s41467-017-01870-0.
Lu, Yu -Jung, Sokhoyan, Ruzan, Cheng, Wen -Hui, Shirmanesh, Ghazaleh Kafaie, Davoyan, Artur R., Pala, Ragip A., Thyagarajan, Krishnan, & Atwater, Harry A. Dynamically controlled Purcell enhancement of visible spontaneous emission in a gated plasmonic heterostructure. United States. doi:10.1038/s41467-017-01870-0.
Lu, Yu -Jung, Sokhoyan, Ruzan, Cheng, Wen -Hui, Shirmanesh, Ghazaleh Kafaie, Davoyan, Artur R., Pala, Ragip A., Thyagarajan, Krishnan, and Atwater, Harry A. Tue . "Dynamically controlled Purcell enhancement of visible spontaneous emission in a gated plasmonic heterostructure". United States. doi:10.1038/s41467-017-01870-0. https://www.osti.gov/servlets/purl/1499680.
@article{osti_1499680,
title = {Dynamically controlled Purcell enhancement of visible spontaneous emission in a gated plasmonic heterostructure},
author = {Lu, Yu -Jung and Sokhoyan, Ruzan and Cheng, Wen -Hui and Shirmanesh, Ghazaleh Kafaie and Davoyan, Artur R. and Pala, Ragip A. and Thyagarajan, Krishnan and Atwater, Harry A.},
abstractNote = {Emission control of colloidal quantum dots (QDs) is a cornerstone of modern high-quality lighting and display technologies. Dynamic emission control of colloidal QDs in an optoelectronic device is usually achieved by changing the optical pump intensity or injection current density. Here we propose and demonstrate a distinctly different mechanism for the temporal modulation of QD emission intensity at constant optical pumping rate. Our mechanism is based on the electrically controlled modulation of the local density of optical states (LDOS) at the position of the QDs, resulting in the modulation of the QD spontaneous emission rate, far-field emission intensity, and quantum yield. We manipulate the LDOS via field effect-induced optical permittivity modulation of an ultrathin titanium nitride (TiN) film, which is incorporated in a gated TiN/SiO2/Ag plasmonic heterostructure. In conclusion, the demonstrated electrical control of the colloidal QD emission provides a new approach for modulating intensity of light in displays and other optoelectronics.},
doi = {10.1038/s41467-017-01870-0},
journal = {Nature Communications},
number = 1,
volume = 8,
place = {United States},
year = {2017},
month = {11}
}

Journal Article:
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Cited by: 19 works
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Figures / Tables:

Fig. 1 Fig. 1 : Concept of gated TiN/SiO2/Ag plasmonic heterostructure for active control of spontaneous emission. a Schematic of the gated plasmonic heterostructure that consists of 80 nm-thick Ag and 9 nm-thick SiO2 layers in which InP quantum dots (QDs) are embedded, followed by a 7 nm layer of TiN. Themore » filling factor of the QDs in SiO2 is 9%. b Cross-sectional transmission electron microscopy image of the fabricated heterostructure. The image shows that the deposited TiN film is conformal and smooth. The scale bar is 10 nm. c High-resolution transmission electron microscopic image of InP QDs with the diameter of 4–5 nm. The PL emission of the QDs peaks at 630 nm. The scale bar is 5 nm. d The proposed physical mechanism of modulation of optical response. When Ag is biased positively (negatively) with respect to TiN, a charge accumulation (depletion) layer is formed in TiN at the TiN/SiO2 interface. Charge accumulation reduces the real part of the dielectric permittivity of the TiN« less

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      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.