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Effect of Interfacial Alloying versus “Volume Scaling” on Auger Recombination in Compositionally Graded Semiconductor Quantum Dots

Journal Article · · Nano Letters
 [1];  [1];  [2];  [2]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of New Mexico, Albuquerque, NM (United States). Center for High Technology Materials (CHTM)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Auger recombination is a nonradiative three-particle process wherein the electron–hole recombination energy dissipates as a kinetic energy of a third carrier. Auger decay is enhanced in quantum-dot (QD) forms of semiconductor materials compared to their bulk counterparts. Because this process is detrimental to many prospective applications of the QDs, the development of effective approaches for suppressing Auger recombination has been an important goal in the QD field. One such approach involves “smoothing” of the confinement potential, which suppresses the intraband transition involved in the dissipation of the electron–hole recombination energy. Here, the present study evaluates the effect of increasing “smoothness” of the confinement potential on Auger decay employing a series of CdSe/CdS-based QDs wherein the core and the shell are separated by an intermediate layer of a CdSexS1–x alloy comprised of 1–5 sublayers with a radially tuned composition. As inferred from single-dot measurements, use of the five-step grading scheme allows for strong suppression of Auger decay for both biexcitons and charged excitons. Further, due to nearly identical emissivities of neutral and charged excitons, these QDs exhibit an interesting phenomenon of lifetime blinking for which random fluctuations of a photoluminescence lifetime occur for a nearly constant emission intensity.
Research Organization:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Organization:
USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
Grant/Contract Number:
AC52-06NA25396
OSTI ID:
1469533
Report Number(s):
LA-UR--17-26004
Journal Information:
Nano Letters, Journal Name: Nano Letters Journal Issue: 9 Vol. 17; ISSN 1530-6984
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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Reducing the Chromaticity Shifts of Light‐Emitting Diodes Using Gradient‐Alloyed Cd x Zn 1− x Se y S 1− y @ZnS Core Shell Quantum Dots with Enhanced High‐Temperature Photoluminescence journal February 2019
Nanostructured colloidal quantum dots for efficient electroluminescence devices journal January 2019
Highly efficient and stable InP/ZnSe/ZnS quantum dot light-emitting diodes journal November 2019
Colloidal semiconductor nanocrystals in energy transfer reactions journal January 2019
Towards the commercialization of colloidal quantum dot solar cells: perspectives on device structures and manufacturing journal January 2020
The effects of discrete and gradient mid-shell structures on the photoluminescence of single InP quantum dots journal January 2019
Insights on heterogeneity in blinking mechanisms and non-ergodicity using sub-ensemble statistical analysis of single quantum-dots journal August 2019
Effects of interface-potential smoothness and wavefunction delocalization on Auger recombination in colloidal CdSe-based core/shell quantum dots journal December 2019
Perspective: Toward highly stable electroluminescent quantum dot light-emitting devices in the visible range journal January 2020