Role of Interface Chemistry in Opening New Radiative Pathways in InP/CdSe Giant Quantum Dots with Blinking-Suppressed Two-Color Emission

Dennis, Allison M.; Buck, Matthew R.; Wang, Feng; Hartmann, Nicolai F.; Majumder, Somak; Casson, Joanna L.; Watt, John Daniel; Doorn, Stephen K.; Htoon, Han; Sykora, Milan; Hollingsworth, Jennifer Ann

doi:10.1002/adfm.201809111

Title: Role of Interface Chemistry in Opening New Radiative Pathways in InP/CdSe Giant Quantum Dots with Blinking-Suppressed Two-Color Emission

Journal Article · Mon Jun 24 00:00:00 EDT 2019 · Advanced Functional Materials

DOI:https://doi.org/10.1002/adfm.201809111· OSTI ID:1569573

Dennis, Allison M. ^[1]; Buck, Matthew R. ^[2]; Wang, Feng ^[3]; Hartmann, Nicolai F. ^[3]; Majumder, Somak ^[4]; Casson, Joanna L. ^[3];

^[3];

^[3]; Sykora, Milan ^[5];

^[3]

Boston Univ., Boston, MA (United States)
United States Naval Academy, Annapolis, MD (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Center for Integrated NanotechnologiesMaterials Physics and Applications DivisionLos Alamos National Laboratory Los Alamos NM 87545 USA
Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Comenius Univ., Bratislava (Slovakia)

Abstract InP/CdSe core/thick‐shell “giant” quantum dots (gQDs) that exhibit blinking‐suppressed two‐color excitonic emission have been synthesized and optically characterized. These type II heterostructures exhibit photoluminescence from both a charge‐separated, near‐infrared type II excitonic state, and a shell‐localized visible‐color excitonic state. Infrared emission is intrinsic to the type II QD, while visible emission can either be eliminated or enhanced through chemical modification of the InP surface prior to CdSe shell growth. Single‐QD photoluminescence measurements confirm that the dual color emission is from individual nanocrystals. The probability of observing dual emission from individual QDs and the extent of blinking suppression increases with shell thickness. Visible emission can be stabilized by the addition of a second shell of CdS, where the resulting InP/CdSe/CdS core/shell/shell nanocrystals afford the strongest blinking suppression, determined by analysis of the Mandel Q parameter. Transient absorption spectroscopy verifies that dual emission arises when hole relaxation from the shell to the core is impeded, possibly as a result of enhanced interfacial hole trapping at F ⁻ or O ²⁻ defect sites. Electron–hole recombination in the shell then competes with slower type II recombination, providing a different mechanism for breaking Kasha's rule and allowing two colors of light to be emitted from one nanostructure.

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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); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Building Technologies Office

Grant/Contract Number:: 89233218CNA000001; 2009LANL1096

OSTI ID:: 1569573

Alternate ID(s):: OSTI ID: 1529019

Report Number(s):: LA-UR-18-28614

Journal Information:: Advanced Functional Materials, Vol. 29, Issue 37; ISSN 1616-301X

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 7 works

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Title: Role of Interface Chemistry in Opening New Radiative Pathways in InP/CdSe Giant Quantum Dots with Blinking-Suppressed Two-Color Emission

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