Dual-Emitting Dot-in-Bulk CdSe/CdS Nanocrystals with Highly Emissive Core- and Shell-Based Trions Sharing the Same Resident Electron
Abstract
Colloidal CdSe nanocrystals (NCs) overcoated with an ultrathick CdS shell, also known as dot-in-bulk (DiB) structures, can support two types of excitons, one of which is core-localized and the other, shell-localized. In the case of weak “sub-single-exciton” pumping, emission alternates between the core- and shell-related channels, which leads to two-color light. This property makes these structures uniquely suited for a variety of photonic applications as well as ideal model systems for realizing complex excitonic quasi-particles that do not occur in conventional core/shell NCs. Furthermore, we show that the DiB design can enable an unusual regime in which the same long-lived resident electron can endow trionlike characteristics to either of the two excitons of the DiB NC (core- or shell-based). These two spectrally distinct trion states are apparent in the measured photoluminescence (PL) and spin dynamics of core and shell excitons conducted over a wide range of temperatures and applied magnetic fields. Low-temperature PL measurements indicate that core- and shell-based trions are characterized by a nearly ideal (~100%) emission quantum yield, suggesting the strong suppression of Auger recombination for both types of excitations. Polarization-resolved PL experiments in magnetic fields of up to 60 T reveal that the core- and the shell-localizedmore »
- Authors:
-
- Univ. degli Studi di Milano-Bicocca, Milano (Italy)
- Technische Univ. Dortmund (Germany)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Technische Univ. Dortmund (Germany); Russian Academy of Science, St. Petersburg (Russia)
- Publication Date:
- Research Org.:
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Science Foundation (NSF)
- OSTI Identifier:
- 1599032
- Report Number(s):
- LA-UR-19-24533
Journal ID: ISSN 1530-6984; TRN: US2103412
- Grant/Contract Number:
- 89233218CNA000001; 20200213DR; DMR-1644779
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nano Letters
- Additional Journal Information:
- Journal Volume: 19; Journal Issue: 12; Journal ID: ISSN 1530-6984
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS; high magnetic field science; nanocrystals; core/shell heterostructures; dual emission; spin dynamics; charged excitons/trions; excitons; Cadmium sulfide; magnetic properties; quantum mechanics; Cadmium selenide
Citation Formats
Pinchetti, Valerio, Shornikova, Elena V., Qiang, Gang, Bae, Wan Ki, Meinardi, Francesco, Crooker, Scott A., Yakovlev, Dmitri R., Bayer, Manfred, Klimov, Victor Ivanovich, and Brovelli, Sergio. Dual-Emitting Dot-in-Bulk CdSe/CdS Nanocrystals with Highly Emissive Core- and Shell-Based Trions Sharing the Same Resident Electron. United States: N. p., 2019.
Web. doi:10.1021/acs.nanolett.9b03676.
Pinchetti, Valerio, Shornikova, Elena V., Qiang, Gang, Bae, Wan Ki, Meinardi, Francesco, Crooker, Scott A., Yakovlev, Dmitri R., Bayer, Manfred, Klimov, Victor Ivanovich, & Brovelli, Sergio. Dual-Emitting Dot-in-Bulk CdSe/CdS Nanocrystals with Highly Emissive Core- and Shell-Based Trions Sharing the Same Resident Electron. United States. https://doi.org/10.1021/acs.nanolett.9b03676
Pinchetti, Valerio, Shornikova, Elena V., Qiang, Gang, Bae, Wan Ki, Meinardi, Francesco, Crooker, Scott A., Yakovlev, Dmitri R., Bayer, Manfred, Klimov, Victor Ivanovich, and Brovelli, Sergio. Fri .
"Dual-Emitting Dot-in-Bulk CdSe/CdS Nanocrystals with Highly Emissive Core- and Shell-Based Trions Sharing the Same Resident Electron". United States. https://doi.org/10.1021/acs.nanolett.9b03676. https://www.osti.gov/servlets/purl/1599032.
@article{osti_1599032,
title = {Dual-Emitting Dot-in-Bulk CdSe/CdS Nanocrystals with Highly Emissive Core- and Shell-Based Trions Sharing the Same Resident Electron},
author = {Pinchetti, Valerio and Shornikova, Elena V. and Qiang, Gang and Bae, Wan Ki and Meinardi, Francesco and Crooker, Scott A. and Yakovlev, Dmitri R. and Bayer, Manfred and Klimov, Victor Ivanovich and Brovelli, Sergio},
abstractNote = {Colloidal CdSe nanocrystals (NCs) overcoated with an ultrathick CdS shell, also known as dot-in-bulk (DiB) structures, can support two types of excitons, one of which is core-localized and the other, shell-localized. In the case of weak “sub-single-exciton” pumping, emission alternates between the core- and shell-related channels, which leads to two-color light. This property makes these structures uniquely suited for a variety of photonic applications as well as ideal model systems for realizing complex excitonic quasi-particles that do not occur in conventional core/shell NCs. Furthermore, we show that the DiB design can enable an unusual regime in which the same long-lived resident electron can endow trionlike characteristics to either of the two excitons of the DiB NC (core- or shell-based). These two spectrally distinct trion states are apparent in the measured photoluminescence (PL) and spin dynamics of core and shell excitons conducted over a wide range of temperatures and applied magnetic fields. Low-temperature PL measurements indicate that core- and shell-based trions are characterized by a nearly ideal (~100%) emission quantum yield, suggesting the strong suppression of Auger recombination for both types of excitations. Polarization-resolved PL experiments in magnetic fields of up to 60 T reveal that the core- and the shell-localized trions exhibit remarkably similar spin dynamics, which in both cases are controlled by spin-flip processes involving a heavy hole.},
doi = {10.1021/acs.nanolett.9b03676},
journal = {Nano Letters},
number = 12,
volume = 19,
place = {United States},
year = {Fri Oct 25 00:00:00 EDT 2019},
month = {Fri Oct 25 00:00:00 EDT 2019}
}
Web of Science
Figures / Tables:
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