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Role of Atomic Stru...
Role of Atomic Structure on Exciton Dynamics and Photoluminescence in NIR Emissive InAs/InP/ZnSe Quantum Dots
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- Enright, Michael J. (author)
- Univ Illinois, Dept Chem, Urbana, IL 61801 USA.;Western Washington Univ, Dept Chem, Bellingham, WA 98225 USA.
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- Jasrasaria, Dipti (author)
- Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA.
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- Hanchard, Mathilde M. (author)
- Univ Illinois, Dept Chem, Urbana, IL 61801 USA.
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- Needell, David R. (author)
- CALTECH, Dept Appl Phys & Mat Sci, Pasadena, CA 91125 USA.
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- Phelan, Megan E. (author)
- CALTECH, Dept Appl Phys & Mat Sci, Pasadena, CA 91125 USA.
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- Weinberg, Daniel (author)
- Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA.;Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA.
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- McDowell, Brinn E. (author)
- Univ Illinois, Dept Chem, Urbana, IL 61801 USA.
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- Hsiao, Haw-Wen (author)
- Univ Illinois, Dept Mat Sci & Engn, Urbana, IL 61801 USA.
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- Akbari, Hamidreza (author)
- CALTECH, Dept Appl Phys & Mat Sci, Pasadena, CA 91125 USA.
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- Kottwitz, Matthew (author)
- Univ Illinois, Dept Chem, Urbana, IL 61801 USA.
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- Potter, Maggie M. (author)
- Univ Illinois, Dept Chem & Biomol Engn, Urbana, IL 61801 USA.
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- Wong, Joeson (author)
- CALTECH, Dept Appl Phys & Mat Sci, Pasadena, CA 91125 USA.
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- Zuo, Jian-Min (author)
- Univ Illinois, Dept Mat Sci & Engn, Urbana, IL 61801 USA.
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- Atwater, Harry A. (author)
- CALTECH, Dept Appl Phys & Mat Sci, Pasadena, CA 91125 USA.
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- Rabani, Eran (author)
- Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA.;Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA.;Tel Aviv Univ, Sackler Ctr Computat Mol & Mat Sci, IL-69978 Tel Aviv, Israel.
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- Nuzzo, Ralph G. (author)
- KTH,Yt- och korrosionsvetenskap,Univ Illinois, Dept Chem, Urbana, IL 61801 USA.
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Univ Illinois, Dept Chem, Urbana, IL 61801 USA;Western Washington Univ, Dept Chem, Bellingham, WA 98225 USA. Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA. (creator_code:org_t)
- 2022-04-26
- 2022
- English.
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In: The Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 126:17, s. 7576-7587
- Related links:
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https://doi.org/10.1...
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https://urn.kb.se/re...
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Abstract
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- The development of bright, near-infrared-emissive quantum dots (QDs) is a necessary requirement for the realization of important new classes of technology. Specifically, there exist significant needs for brighter, heavy metal-free, near-infrared (NIR) QDs for applications with high radiative efficiency that span diverse applications, including down-conversion emitters for high-performance luminescent solar concentrators. We use a combination of theoretical and experimental approaches to synthesize bright, NIR luminescent InAs/InP/ZnSe QDs and elucidate fundamental material attributes that remain obstacles for development of near-unity NIR QD luminophores. First, using Monte Carlo ray tracing, we identify the atomic and electronic structural attributes of InAs core/shell, NIR emitters, whose luminescence properties can be tailored by synthetic design to match most beneficially those of high-performance, single-band-gap photovoltaic devices based on important semiconductor materials, such Si or GaAs. Second, we synthesize InAs/InP/ZnSe QDs based on the optical attributes found to maximize LSC performance and develop methods to improve the emissive qualities of NIR emitters with large, tunable Stokes ratios, narrow emission linewidths, and high luminescence quantum yields (here reaching 60 +/- 2%). Third, we employ atomistic electronic structure calculations to explore charge carrier behavior at the nanoscale affected by interfacial atomic structures and find that significant exciton occupation of the InP shell occurs in most cases despite the InAs/InP type I bulk band alignment. Furthermore, the density of the valence band maximum state extends anisotropically through the (111) crystal planes to the terminal InP surfaces/interfaces, indicating that surface defects, such as unpassivated phosphorus dangling bonds, located on the (111) facets play an outsized role in disrupting the valence band maximum and quenching photoluminescence.
Subject headings
- NATURVETENSKAP -- Kemi -- Fysikalisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Physical Chemistry (hsv//eng)
Publication and Content Type
- ref (subject category)
- art (subject category)
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Enright, Michael ...
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Jasrasaria, Dipt ...
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Hanchard, Mathil ...
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Needell, David R ...
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Phelan, Megan E.
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Weinberg, Daniel
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McDowell, Brinn ...
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Hsiao, Haw-Wen
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Akbari, Hamidrez ...
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Kottwitz, Matthe ...
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Potter, Maggie M ...
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Wong, Joeson
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Zuo, Jian-Min
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Atwater, Harry A ...
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Rabani, Eran
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Nuzzo, Ralph G.
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- NATURAL SCIENCES
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NATURAL SCIENCES
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and Physical Chemist ...
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The Journal of P ...
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Royal Institute of Technology