Browsing by Subject "Auger recombination"
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Item Open Access Blue liquid lasers from solution of CdZnS/ZnS ternary alloy quantum dots with quasi ‐ continuous pumping(Wiley - VCH Verlag GmbH & Co. KGaA, 2015) Wang Y.; Leck K.S.; Ta, V. D.; Chen R.; Nalla, V.; Gao, Y.; He T.; Demir, Hilmi Volkan; Sun, H.A blue (ca. 440 nm) liquid laser with an ultra‐low threshold through which quasi‐continuous wave pumping is accessible is achieved by engineering unconventional ternary CdZnS/ZnS alloyed‐core/shell QDs. Such an achievement is enabled by exploiting the novel gain media with minimal defects, suppressed Auger recombination, and large gain cross‐section in combination with high‐quality‐factor whispering gallery mode resonators.Item Open Access Electrically control amplified spontaneous emission in colloidal quantum dots(American Association for the Advancement of Science, 2019) Yu, J.; Shendre, S.; Koh, W.; Liu, B.; Li, M.; Hou, S.; Hettiarachchi, C.; Delikanlı, S.; Hernandez-Martinez, P.; Birowosuto, M. D.; Wang, H.; Sum, T.; Demir, Hilmi Volkan; Dang, C.Colloidal quantum dots (CQDs) are highly promising materials for light amplification thanks to their efficient photoluminescence, tunable emission wavelength and low-cost synthesis. Unfortunately, CQDs are suffering from band-edge state degeneracy which demands multiple excitons to achieve population inversion. As a result, non-radiative Auger recombination increases the lasing threshold and limits the gain lifetime. Here, benefiting from the negative charging, we demonstrate that the amplified spontaneous emission (ASE) threshold is controllable in a device where CQD film is exposed to an external electric field. Specifically, singly charged CQDs lower the threshold due to the preexisting electron in the conduction band, while strongly enhanced Auger recombination in doubly charged CQDs stymies the ASE. Experimental results and kinetic equation model show that ASE threshold reduces 10% even if our device only charges ~17% of the CQD population. Our results open new possibilities for controlling exciton recombination dynamics and achieving electrically pumped CQD lasers.Item Open Access Exciton dynamics in colloidal quantum-dot LEDs under active device operations(American Chemical Society, 2018) Shendre, S.; Sharma, V. K.; Dang C.; Demir, Hilmi VolkanColloidal quantum-dot light-emitting diodes (QLEDs) are lucrative options for color-pure lighting sources. To achieve high-performance QLEDs, besides developing high-efficiency quantum dots (QDs), it is essential to understand their device physics. However, little understanding of the QD emission behavior in active QLEDs is one of the main factors hindering the improvement of device efficiency. In this work, we systematically studied the exciton dynamics of gradient composition CdSe@ZnS QDs during electroluminescence in a working QLED. With time-resolved photoluminescence analyses using fluorescence lifetime imaging microscopy we analyzed a large population of QDs spatially spreading over an extended area inside and outside the device. This allows us to reveal the statistically significant changes in the behavior of QD emission in the device at different levels of applied voltages and injection currents. We find that the QD emission efficiency first drops in device fabrication with Al electrode deposition and that the QD exciton lifetime is then statistically reduced further under the QLED's working conditions. This implies the nonradiative Auger recombination process is active in charged QDs as a result of imbalanced charge injection in a working QLED. Our results help to understand the exciton behavior during the operation of a QLED and demonstrate a new approach to explore the exciton dynamics statistically with a large QD population.Item Open Access Giant alloyed hot injection shells enable ultralow optical gain threshold in colloidal quantum wells(American Chemical Society, 2019) Altıntaş, Yemliha; Güngör, Kıvanç; Gao, Y.; Sak, Mustafa; Quliyeva, Ulviyya; Bappi, G.; Mutlugün, Evren; Sargent, E. H.; Demir, Hilmi VolkanAs an attractive materials system for high-performance optoelectronics, colloidal nanoplatelets (NPLs) benefit from atomic-level precision in thickness, minimizing emission inhomogeneous broadening. Much progress has been made to enhance their photoluminescence quantum yield (PLQY) and photostability. However, to date, layer-by-layer growth of shells at room temperature has resulted in defects that limit PLQY and thus curtail the performance of NPLs as an optical gain medium. Here, we introduce a hot-injection method growing giant alloyed shells using an approach that reduces core/shell lattice mismatch and suppresses Auger recombination. Near-unity PLQY is achieved with a narrow full-width-at-half-maximum (20 nm), accompanied by emission tunability (from 610 to 650 nm). The biexciton lifetime exceeds 1 ns, an order of magnitude longer than in conventional colloidal quantum dots (CQDs). Reduced Auger recombination enables record-low amplified spontaneous emission threshold of 2.4 μJ cm–2under one-photon pumping. This is lower by a factor of 2.5 than the best previously reported value in nanocrystals (6 μJ cm–2 for CdSe/CdS NPLs). Here, we also report single-mode lasing operation with a 0.55 mJ cm–2 threshold under two-photoexcitation, which is also the best among nanocrystals (compared to 0.76 mJ cm–2 from CdSe/CdS CQDs in the Fabry–Pérot cavity). These findings indicate that hot-injection growth of thick alloyed shells makes ultrahigh performance NPLs.Item Open Access Near-unity efficiency energy transfer from colloidal semiconductor quantum wells of CdSe/cdS nanoplatelets to a monolayer of MoS2(American Chemical Society, 2018) Taghipour, N.; Martinez, P. L. H.; Ozden, A.; Olutas M.; Dede, D.; Gungor K.; Erdem, O.; Perkgoz, N. K.; Demir, Hilmi VolkanA hybrid structure of the quasi-2D colloidal semiconductor quantum wells assembled with a single layer of 2D transition metal dichalcogenides offers the possibility of highly strong dipole-to-dipole coupling, which may enable extraordinary levels of efficiency in Förster resonance energy transfer (FRET). Here, we show ultrahigh-efficiency FRET from the ensemble thin films of CdSe/CdS nanoplatelets (NPLs) to a MoS2 monolayer. From time-resolved fluorescence spectroscopy, we observed the suppression of the photoluminescence of the NPLs corresponding to the total rate of energy transfer from ∼0.4 to 268 ns-1. Using an Al2O3 separating layer between CdSe/CdS and MoS2 with thickness tuned from 5 to 1 nm, we found that FRET takes place 7- to 88-fold faster than the Auger recombination in CdSe-based NPLs. Our measurements reveal that the FRET rate scales down with d-2 for the donor of CdSe/CdS NPLs and the acceptor of the MoS2 monolayer, d being the center-to-center distance between this FRET pair. A full electromagnetic model explains the behavior of this d-2 system. This scaling arises from the delocalization of the dipole fields in the ensemble thin film of the NPLs and full distribution of the electric field across the layer of MoS2. This d-2 dependency results in an extraordinarily long Förster radius of ∼33 nm.Item Open Access Stable and low ‐ threshold optical gain in CdSe/CdS quantum dots: an all ‐ colloidal frequency up ‐ converted laser(Wiley-VCH Verlag, 2015) Güzeltürk, B.; Keleşemur, Y.; Güngor, K.; Yeltik, A.; Akgül, M. Z.; Wang, Y.; Chen R.; Dang, C.; Sun, H.; Demir, Hilmi VolkanAn all-solution processed and all-colloidal laser is demonstrated using tailored CdSe/CdS core/shell quantum dots, which exhibit highly stable and low-threshold optical gain owing to substantially suppressed non-radiative Auger recombination.Item Open Access Unraveling the ultralow threshold stimulated emission from CdZnS/ZnS quantum dot and enabling high ‐ Q microlasers(Wiley-VCH Verlag, 2015) Wang Y.; Fong, K. E.; Yang, S.; Ta, V.; Gao, Y.; Wang, Z.; Nalla, V.; Demir, Hilmi Volkan; Sun, H.The newly engineered ternary CdZnS/ZnS colloidal quantum dots (CQDs) are found to exhibit remarkably high photoluminescence quantum yield and excellent optical gain properties. However, the underlying mechanisms, which could offer the guidelines for devising CQDs for optimized photonic devices, remain undisclosed. In this work, through comprehensive steady-state and time-resolved spectroscopy studies on a series of CdZnS-based CQDs, we unambiguously clarify that CdZnS-based CQDs are inherently superior optical gain media in the blue spectral range due to the slow Auger process and that the ultralow threshold stimulated emission is enabled by surface/interface engineering. Furthermore, external cavity-free high-Q quasitoroid microlasers were produced from self-assembly of CdZnS/ZnS CQDs by facile inkjet printing technique. Detailed spectroscopy analysis confirms the whispering gallery mode lasing mechanism of the quasitoroid microlasers. This tempting microlaser fabrication method should be applicable to other solution-processed gain materials, which could trigger broad research interests. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA.