The development of nanocrystal quantum dots (NQDs) with suppressed nonradiative Auger recombination has been an important goal in colloidal nanostructure research motivated by the needs of prospective applications in lasing devices, light-emitting diodes, and photovoltaic cells. Here, we conduct single-nanocrystal spectroscopic studies of recently developed core-shell NQDs (so-called "giant" NQDs) that comprise a small CdSe core surrounded by a 16-monolayer-thick CdS shell. Using both continuous-wave and pulsed excitation, we observe strong emission features due both to neutral and charged biexcitons, as well as multiexcitons of higher order. The development of pronounced multiexcitonic peaks in steady-state photoluminescence of individual nanocrystals, as well as continuous growth of the emission intensity in the range of high pump levels, point toward a significant suppression of nonradiative Auger decay that normally renders multiexcitons nonemissive. The unusually high multiexciton emission efficiencies in these systems open interesting opportunities for studies of multiexciton phenomena using well-established methods of single-dot spectroscopy, as well as new exciting prospects for applications, that have previously been hampered by nonradiative Auger decay.
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http://dx.doi.org/10.1021/nl1004652 | DOI Listing |
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January 2025
College of Physics and Optoelectronic Engineering, Harbin Engineering University, Harbin, 150001, P. R. China.
Currently, CsPbI quantum dots (QDs) based light-emitting diodes (LEDs) are not well suited for achieving high efficiency and operational stability due to the binary-precursor method and purification process, which often results in the nonstoichiometric ratio of Cs/Pb/I. This imbalance leads to amounts of iodine vacancies, inducing severe non-radiative recombination processes and phase transitions of QDs. Herein, red-emitting CsPbI QDs are reported with excellent optoelectronic properties and stability based on the synergistic effects of halide-rich modulation passivation and lattice repair.
View Article and Find Full Text PDFNanoscale
January 2025
The Canter for Photochemical Sciences and Department of Physics, Bowling Green State University, Bowling Green, Ohio 43403, USA.
Laser diodes based on solution-processed semiconductor quantum dots (QDs) present an economical and color-tunable alternative to traditional epitaxial lasers. However, their efficiency is significantly limited by non-radiative Auger recombination, a process that increases lasing thresholds and diminishes device longevity through excessive heat generation. Recent advancements indicate that these limitations can be mitigated by employing spherical quantum wells, or quantum shells (QSs), in place of conventional QDs.
View Article and Find Full Text PDFAdv Mater
December 2024
Experimental Center of Advanced Materials, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081, China.
Anisotropic nanoplatelets (NPLs) possess strong in-plane transition dipole moments and out-of-plane emission, which enable a maximum photon out-coupling efficiency of 40% and a high gain coefficient, making them ideal candidates for light-emitting diodes (LEDs) and lasers. However, the unbalanced surface energy between the side and top facets of NPLs results in poor thermal stability and high susceptibility to ripening at elevated temperatures, which complicates the growth of the shell. To address this issue, a gradient crown (CdSeS) around the CdSe NPLs is designed to stabilize the high energy side facets.
View Article and Find Full Text PDFJ Phys Condens Matter
December 2024
Tyndall National Institute, University College Cork, Cork T12 R5CP, Ireland.
Nat Mater
January 2025
Nanotechnology and Advanced Spectroscopy Team, C-PCS, Chemistry Division, Los Alamos National Laboratory, Los Alamos, NM, USA.
Present-day liquid-state lasers are based on organic dyes. Here we demonstrate an alternative class of liquid lasers that use solutions of colloidal quantum dots (QDs). Previous efforts to realize such devices have been hampered by the fast non-radiative Auger recombination of multicarrier states required for optical gain.
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