Giant nanocrystal quantum dots: stable down-conversion phosphors that exploit a large stokes shift and efficient shell-to-core energy relaxation

Nano Letters
Janardan KunduJennifer A Hollingsworth

Abstract

A new class of nanocrystal quantum dot (NQD), the "giant" NQD (g-NQD), was investigated for its potential to address outstanding issues associated with the use of NQDs as down-conversion phosphors in light-emitting devices, namely, insufficient chemical/photostability and extensive self-reabsorption when packed in high densities or in thick films. Here, we demonstrate that g-NQDs afford significantly enhanced operational stability compared to their conventional NQD counterparts and minimal self-reabsorption losses. The latter results from a characteristic large Stokes shift (>100 nm; >0.39 eV), which itself is a manifestation of the internal structure of these uniquely thick-shelled NQDs. In carefully prepared g-NQDs, light absorption occurs predominantly in the shell but emission occurs exclusively from the core. We directly compare for the first time the processes of shell→core energy relaxation and core→core energy transfer by evaluating CdS→CdSe down-conversion of blue→red light in g-NQDs and in a comparable mixed-NQD (CdSe and CdS) thin film, revealing that the internal energy relaxation process affords a more efficient and color-pure conversion of blue to red light compared to energy transfer. Lastly, we demonstrate the f...Continue Reading

References

Jun 6, 2000·Journal of Biomolecular Screening·J R LakowiczZ Gryczynski
Mar 22, 2008·Journal of the American Chemical Society·Yongfen ChenJennifer A Hollingsworth
Jun 10, 2009·Nano Letters·Florencio García-SantamaríaVictor I Klimov
Jun 3, 2010·Advanced Materials·Eunjoo JangYounghwan Kim
Jul 6, 2010·Small·Quanqin DaiMichael Z Hu
Oct 12, 2010·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Ákos I FábiánAttila Jenei

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Citations

Sep 26, 2013·Chemistry of Materials : a Publication of the American Chemical Society·Jennifer A Hollingsworth
Dec 21, 2012·Nano Letters·Steven M Hughes, A Paul Alivisatos
Jun 9, 2015·ACS Applied Materials & Interfaces·Christina J HansonJennifer A Hollingsworth
Aug 12, 2015·The Journal of Physical Chemistry Letters·Melissa PauliteHan Htoon
Jun 3, 2014·ACS Nano·Burak GuzelturkHilmi Volkan Demir
Aug 9, 2016·Chemical Reviews·Rachel D HarrisEmily A Weiss
Dec 12, 2012·Langmuir : the ACS Journal of Surfaces and Colloids·Seungho ChoSungjee Kim
Sep 30, 2016·Chemical Reviews·Jeffrey M PietrygaVictor I Klimov
May 13, 2017·Nature Communications·Nimai MishraJennifer A Hollingsworth
Jan 20, 2015·Angewandte Chemie·Ali Hossain KhanSomobrata Acharya
Oct 25, 2017·Nanoscale·Margaret ChernAllison M Dennis
Jan 16, 2019·Applied Optics·Hongyu YangJiayu Zhang
Mar 24, 2015·Advanced Functional Materials·Aaron M KellerJames H Werner
Oct 17, 2019·The Journal of Chemical Physics·Sungjun KohDoh C Lee
Aug 29, 2018·ACS Applied Materials & Interfaces·Michael WorkuBiwu Ma
Jun 12, 2020·ACS Applied Materials & Interfaces·Noah J OrfieldJennifer A Hollingsworth

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