Browsing by Author "Sum, T. C."

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Open Access
Fluorophore-doped core-multishell spherical plasmonic nanocavities: resonant energy transfer towards a loss compensation
(American Chemical Society, 2012-06-12) Peng, B.; Zhang, Q.; Liu, X.; Ji Y.; Demir, Hilmi Volkan; Huan, C. H. A.; Sum, T. C.; Wiong, Q.
Plasmonics exhibits the potential to break the diffraction limit and bridge the gap between electronics and photonics by routing and manipulating light at the nanoscale. However, the inherent and strong energy dissipation present in metals, especially in the near-infrared and visible wavelength ranges, significantly hampersthe applications in nanophotonics. Therefore, it is amajor challengetomitigatethe losses. One way to compensate the losses is to incorporate gain media into plasmonics. Here, we experimentally show that the incorporation of gain material into a local surface plasmonic system (Au/silica/silica dye core multishell nanoparticles) leads to a resonant energy transfer from the gain media to the plasmon. The optimized conditions for the largest loss compensation are reported. Both the coupling distance and the spectral overlap arethe key factorsto determinetheresulting energy transfer. Theinterplay of these factors leadsto a non-monotonous photoluminescence dependence as a function of the silica spacer shell thickness. Nonradiativetransferrate is increased by morethan 3 orders of magnitude attheresonant condition, which is key evidence of the strongest coupling occurring between the plasmon and the gain material.
Open Access
Green stimulated emission boosted by nonradiative resonant energy transfer from blue quantum dots
(American Chemical Society, 2016) Gao, Y.; Yu, G.; Wang Y.; Dang C.; Sum, T. C.; Sun, H.; Demir, Hilmi Volkan
Thanks to their tunability and versatility, the colloidal quantum dots (CQDs) made of II-VI semiconductor compound offer the potential to bridge the "green gap" in conventional semiconductors. However, when the CQDs are pumped to much higher initial excitonic states compared to their bandgap, multiexciton interaction is enhanced, leading to a much higher stimulated emission threshold. Here, to circumvent this drawback, for the first time, we show a fully colloidal gain in green enabled by a partially indirect pumping approach assisted by Förster resonance energy transfer process. By introducing the blue CQDs as exciton donors, the lasing threshold of the green CQDs, is reduced dramatically. The blue CQDs thus serve as an energy-transferring buffer medium to reduce excitation energy from pumping photons in a controlled way by injecting photoinduced excitons into green CQDs. Our newly developed colloidal pumping scheme could enable efficient CQD lasers of full visible colors by a single pump source and cascaded exciton transfer. This would potentially pave the way for an efficient multicolor laser for lighting and display applications.
Open Access
High brightness formamidinium lead bromide perovskite nanocrystal light emitting devices
(Nature Publishing Group, 2016) Perumal, A.; Shendre, S.; Li, M.; Tay, Y. K. E.; Sharma, V. K.; Chen, S.; Wei, Z.; Liu, Q.; Gao, Y.; Buenconsejo, P. J. S.; Tan S.T.; Gan, C. L.; Xiong, Q.; Sum, T. C.; Demir, Hilmi Volkan
Formamidinium lead halide (FAPbX3) has attracted greater attention and is more prominent recently in photovoltaic devices due to its broad absorption and higher thermal stability in comparison to more popular methylammonium lead halide MAPbX3. Herein, a simple and highly reproducible room temperature synthesis of device grade high quality formamidinium lead bromide CH(NH2)2 PbBr3 (FAPbBr3) colloidal nanocrystals (NC) having high photoluminescence quantum efficiency (PLQE) of 55-65% is reported. In addition, we demonstrate high brightness perovskite light emitting device (Pe-LED) with these FAPbBr3 perovskite NC thin film using 2,2′,2″-(1,3,5-Benzinetriyl)-tris(1-phenyl-1-H-benzimidazole) commonly known as TPBi and 4,6-Bis(3,5-di(pyridin-3-yl)phenyl)-2-methylpyrimidine (B3PYMPM) as electron transport layers (ETL). The Pe-LED device with B3PYMPM as ETL has bright electroluminescence of up to 2714 cd/m2, while the Pe-LED device with TPBi as ETL has higher peak luminous efficiency of 6.4 cd/A and peak luminous power efficiency of 5.7 lm/W. To our knowledge this is the first report on high brightness light emitting device based on CH(NH2)2 PbBr3 widely known as FAPbBr3 nanocrystals in literature. © The Author(s) 2016.
Open Access
Low-threshold lasing from colloidal CdSe/CdSeTe core/alloyed-crown type-II heteronanoplatelets
(Royal Society of Chemistry, 2018) Gao, Y.; Li, M.; Delikanli S.; Zheng, H.; Liu, B.; Dang C.; Sum, T. C.; Demir, Hilmi Volkan
Colloidal type-II heterostructures are believed to be a promising solution-processed gain medium given their spatially separated electrons and holes for the suppression of Auger recombination and their wider emission tuning range from the visible to near-infrared region. Amplified spontaneous emission (ASE) was achieved from colloidal type-II core/shell nanocrystals several years ago. However, due to the limited charge-transfer (CT) interfacial states and minimal overlap of electron and hole wave functions, the ASE threshold has still been very high. Herein, we achieved ASE through type-II recombination at a lower threshold using CdSe/CdSeTe core/alloyed-crown nanoplatelets. Random lasing was also demonstrated in the film of these nanoplatelets under sub-ns laser-pumping. Through a detailed carrier dynamics investigation using femtosecond transient absorption, steady state, and time-resolved photoluminescence (PL) spectroscopies, we confirmed the type-II band alignment, and found that compared with normal CdSe/CdTe core/crown nanoplatelets (where no ASE/lasing was observed), CdSe/CdSeTe core/alloyed-crown nanoplatelets had a much higher PL quantum yield (75% vs. 31%), a ∼5-fold larger density of type-II charge-transfer states, a faster carrier transfer to interfaces (0.32 ps vs. 0.61 ps) and a slower Auger recombination lifetime (360 ps vs. 160 ps). Compared with CdSe/CdTe nanoplatelets, their counterparts with an alloyed crown boast a promoted charge transfer process, higher luminescence quantum yield, and smaller Auger rate, which results in their excellent application potential in solution-processed lasers and light-emitting devices.
Open Access
Sub-single exciton optical gain threshold in colloidal semiconductor quantum wells with gradient alloy shelling
(Nature Research, 2020) Taghipour, Nima; Delikanlı, Savaş; Shendre, S.; Sak, Mustafa; Li, M.; Işık, Furkan; Tanrıöver, İbrahim; Güzeltürk, B.; Sum, T. C.; Demir, Hilmi Volkan
Colloidal semiconductor quantum wells have emerged as a promising material platform for use in solution-processable lasers. However, applications relying on their optical gain suffer from nonradiative Auger decay due to multi-excitonic nature of light amplification in II-VI semiconductor nanocrystals. Here, we show sub-single exciton level of optical gain threshold in specially engineered CdSe/CdS@CdZnS core/crown@gradient-alloyed shell quantum wells. This sub-single exciton ensemble-averaged gain threshold of (Ng)≈ 0.84 (per particle) resulting from impeded Auger recombination, along with a large absorption cross-section of quantum wells, enables us to observe the amplified spontaneous emission starting at an ultralow pump fluence of ~ 800 nJ cm−2, at least three-folds better than previously reported values among all colloidal nanocrystals. Finally, using these gradient shelled quantum wells, we demonstrate a vertical cavity surface-emitting laser operating at a low lasing threshold of 7.5 μJ cm−2. These results represent a significant step towards the realization of solution-processable electrically-driven colloidal lasers.
Open Access
Ultrahigh-efficiency aqueous flat nanocrystals of CdSe/CdS@Cd1−xZnxS colloidal core/crown@alloyed-shell quantum wells
(Royal Society of Chemistry, 2019) Shendre, S.; Delikanlı, Savaş; Li, M.; Dede, Didem; Pan, Z.; Ha, S. T.; Fu, Y. H.; Hernández-Martínez, Pedro L.; Yu, J.; Erdem, Onur; Kuznetsov, A. I.; Dang, C.; Sum, T. C.; Demir, Hilmi Volkan
Colloidal semiconductor nanoplatelets (NPLs) are highly promising luminescent materials owing to their exceptionally narrow emission spectra. While high-efficiency NPLs in non-polar organic media can be obtained readily, NPLs in aqueous media suffer from extremely low quantum yields (QYs), which completely undermines their potential, especially in biological applications. Here, we show high-efficiency water-soluble CdSe/CdS@Cd1−xZnxS core/crown@shell NPLs formed by layer-by-layer grown and composition-tuned gradient Cd1−xZnxS shells on CdSe/CdS core/crown seeds. Such control of shell composition with monolayer precision and effective peripheral crown passivation, together with the compact capping density of short 3-mercaptopropionic acid ligands, allow for QYs reaching 90% in water, accompanied by a significantly increased photoluminescence lifetime (∼35 ns), indicating the suppression of nonradiative channels in these NPLs. We also demonstrate the controlled attachment of these NPLs without stacking at the nanoscale by taking advantage of their 2D geometry and hydrophilicity. This is a significant step in achieving controlled assemblies and overcoming the stacking process, which otherwise undermines their film formation and performance in optoelectronic applications. Moreover, we show that the parallel orientation of such NPLs achieved by the controlled attachment enables directed emission perpendicular to the surface of the NPL films, which is highly advantageous for light extraction in light-emitting platforms..