Dual-Emitting Dot-in-Bulk CdSe/CdS Nanocrystals with Highly Emissive Core- and Shell-Based Trions Sharing the Same Resident Electron

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

doi:10.1021/acs.nanolett.9b03676

Title: Dual-Emitting Dot-in-Bulk CdSe/CdS Nanocrystals with Highly Emissive Core- and Shell-Based Trions Sharing the Same Resident Electron

Journal Article · Fri Oct 25 00:00:00 EDT 2019 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.9b03676· OSTI ID:1599032

^[1];

^[2]; Qiang, Gang ^[2]; Bae, Wan Ki ^[3]; Meinardi, Francesco ^[1];

^[3];

^[4]; Bayer, Manfred ^[4];

^[3];

^[1]

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)

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.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Science Foundation (NSF)

Grant/Contract Number:: 89233218CNA000001; 20200213DR; DMR-1644779

OSTI ID:: 1599032

Report Number(s):: LA-UR-19-24533; TRN: US2103412

Journal Information:: Nano Letters, Vol. 19, Issue 12; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 4 works

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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

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