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Title: 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 » trions exhibit remarkably similar spin dynamics, which in both cases are controlled by spin-flip processes involving a heavy hole.« less

Authors:
ORCiD logo [1]; ORCiD logo [2];  [2];  [3];  [1]; ORCiD logo [3]; ORCiD logo [4];  [4]; ORCiD logo [3]; ORCiD logo [1]
  1. Univ. degli Studi di Milano-Bicocca, Milano (Italy)
  2. Technische Univ. Dortmund (Germany)
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  4. Technische Univ. Dortmund (Germany); Russian Academy of Science, St. Petersburg (Russia)
Publication Date:
Research Org.:
Los Alamos National Laboratory (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 = {2019},
month = {10}
}

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Figures / Tables:

Figure 1 Figure 1: (a) Energy band diagram of a DiB NCs featuring a CdSe core with the zincblende (ZB) structure (red) overcoated with an epitaxial layer of CdS in the ZB phase (dark green), followed by a thick shell of CdS with the wurtzite (WZ) structure (light green). The core andmore » shell excitons are also depicted. (b) Schematics of the formation of negative trions in the CdSe core (middle) and the CdS shell (right) upon photo-excitation of a negatively charged DiB NC (left). The core (shell) trions consist of the core (shell) exciton interacting with the resident electron (patterned filling). Since after thermalization the resident electron and the photoelectron occupy the same quantized state at the conduction band edge, the spin state of the photoelectron is dictated by the spin projection of the resident electron (assumed here to be a spin-up state), which is a direct consequence of the Pauli exclusion principle. The photo-hole can, in principle, reside in either of the spin states (up or down). (c) Schematic representation of the spin level structures and the optical transitions for a negative trion comprising a heavy hole in a magnetic field. Double- and single-line short black arrows indicate hole and electron spins, respectively. Polarized optical transitions are shown by red ($σ$+) and blue ($σ$) arrows. The more intense emission, shown by the thicker blue arrow, originates from the lower-energy trion state with spin −3/2.« less

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