Browsing by Subject "Colloidal quantum wells"
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Item Open Access Colloidal optoelectronics of self-assembled quantum well superstructures(Bilkent University, 2020-06) Erdem, OnurAdvances in the colloidal nanocrystal synthesis enabled creation of quasi twodimensional colloidal quantum wells (CQWs) in the last decade. These CQWs possess similar properties to those of epitaxially grown quantum wells while at the same time offering the benefits of low-cost synthesis and solubility in various solvents. Their atomically precise thickness and one-dimensional quantum confinement grant them favorable properties such as narrow emission linewidth, reduced inhomogeneous broadening and giant oscillator strength. In addition, due to their quasi-two dimensional shape, they display intrinsic anisotropy. Because of this anisotropy, the particle interactions in closely packed films depend greatly on the orientation of these CQWs. To fully utilize the interaction of CQWs with each other or with other particles in their proximity, we develop a selfassembly technique, which is used to deposit highly uniform thin CQW films onto various solid substrates. This self-assembly technique allows us to deposit CQWs as a continuous monolayer while at the same time controlling their orientation throughout the substrate, thereby modifying their packing factor as well as nearfield dipole-dipole interactions. This self-assembly technique is also employed to create large-area CQW films of any desired thickness, simply by applying the same deposition technique on the same substrate as many times as desired. We use these self-assembled CQW films to study the two main aspects of nanocrystal optoelectronics, namely, Förster resonance energy transfer (FRET) and optical gain, with CQWs. By using the orientation-controlled CQW monolayers, we show that the rate of FRET from colloidal quantum dots (QDs) to a monolayer of CQWs can be tuned via dipole-dipole interactions between QDs and CQWs. We use Förster’s theory of nonradiative energy transfer while taking into account the anisotropy of the excitonic CQW excitonic state as well as its delocalization throughout the CQW to account for our results. Next, we show that our multilayered CQW films display optical gain in uncharacteriscally low thicknesses (as small as 40 nm) due to the tight packing and extremely uniform deposition of the CQWs. We furthermore study systematically the observed threshold of amplified spontaneous emission (ASE) in these CQW multilayers as a function of the film thickness (i.e., the number of monolayers), and demonstrate that the gain threshold drops with increasing thickness, accompanied by the red-shift of the ASE peak. These trends can be explained by the varying degree of optical mode confinement, which is a function of both the film thickness as well as the wavelength of propagating mode. Our self-assembly technique allows to study and make use of the favorable properties of the CQWs including anisotropy and enhanced optical gain. Since this technique enables us to produce large-area films displaying excellent homogeneity, it can be a benchmark building block for creating device-scale 2- or 3-dimensional superstructures from CQWs as well as from other types of colloidal nanocrystals to be utilized in both in- and out-of-plane optical applications.Item Open Access Colloidal quantum well light-emitting waveguides(Bilkent University, 2023-07) Işık, Ahmet TarıkMicro/nanoscale semiconductor light-emitting devices of colloidal nanocrystals offer low-cost solutions while delivering high performance in ambient lighting systems, displays, and photonic circuits. Colloidal quantum wells (CQWs) are excellent candidates as active materials for these optoelectronic devices owing to their superior properties including suppressed Auger recombination, large absorption cross-section, and narrow emission linewidth. In this thesis, as our first study, we proposed and demonstrated dual-color lasing using heterostructures of CQWs as the gain media in an all-solution-processed dual-color optical cavity for the first time. Here, a multilayered waveguide architecture consisting of green- and red-emitting CQWs, separated with a transparent low refractive index colloidal spacing layer of silica nanoparticles (NPs) suppressing otherwise detrimental nonradiative energy transfer between them, enabled amplified spontaneous emission (ASE) simultaneously in two colors at the threshold level of ~17 µJ/cm2 . We further adapted this multilayer waveguide configuration to a whispering-gallery-mode (WGM) cavity by fabricating a microdisk structure directly out of these layered CQWs-NPs-CQWs colloids. The resulting device showed dual-color multimode lasing both at 569 and 648 nm at the same time with the threshold of ~106 µJ/cm2 . Then, as the second study of this thesis, we developed a colloidal waveguide light-emitting diode (LED) structure of CQWs that changes the direction of light from the surface to the edge of the device by combining the active CQW region with a slit-shaped waveguide architecture that confines the light within the emissive layer and guides it through the lateral axis. Driving this LED waveguide of 900 µm in length by 150 µm in width at a current density level of 5.6 A/cm2 , we observed the output emission reached a luminance level of ~20,400 cd/m2 . These unique waveguiding architectures integrated into the light emitting devices of CQWs hold great promise for on-chip photonic applications including CQW dual-color excitation for biological imaging and CQW LED-based photonic integrated circuits.Item Open Access Colloidal synthesis and doping of semiconductor nanocrystals(Bilkent University, 2015-07) Akgül, Mehmet ZaferColloidal semiconductor nanocrystals have drawn great interest for application areas in photonics and optoelectronics thanks to their superior optical properties including strong bandgap emission and tunability. Also, their suitability for solution-based processing has made them highly attractive for low-cost production of light-emitting diodes and lasers. Our objective in this thesis is to show the potential and versatility of semiconductor nanocrystals via colloidal synthesis and post-processing methods. The thesis work includes the synthesis of colloidal quantum dot and well structures and their post-doping and investigates their exciton decay dynamics. In this thesis a novel colloidal approach for the doping of zinc blende colloidal quantum wells was proposed and demonstrated for the first time. This new doping method uniquely relies on atomic layer deposition (ALD) process. Here we achieved the worlds first manganese-doped CdSe@CdS core@shell nanoplatelets using our technique of ALD-assisted doping. Also, we studied silver-doped CdTe quantum dots under different conditions. Our experimental work proved that the quantum yield enhancement of silver-doped CdTe quantum dots is a strong function of the nanocrystal size and doping concentration. Tuning the nanocrystal size and doping level, our aqueous core-only CdTe nanocrystals reached a record high photoluminescence quantum efficiency of 68%. For these quantum dots, various decay kinetics were proposed and the enhancement in the quantum yield was attributed to the trap state annihilation. The methods and results provided in this thesis contribute to the fundamental understanding of semiconductornanocrystals and pave the way for high-performance colloidal platforms and devices.Item Embargo Colloidal synthetic pathways of atomically-flat complex nanocrystal heterostructures(Bilkent University, 2024-01) Shabani, FarzanColloidal semiconductor nanocrystals (NCs) constitute one of the most important branches of nanoscience, with an increasingly high research interest, culminating with a Nobel Prize most recently. The nanometric size of these NCs allows for size-dependent optical properties, which provides an extra tool besides the composition to fine-tune these properties. Recent advancements in NC synthesis have been enabling important developments in the design and engineering of different shapes, compositions, and heterostructures of NCs. Accompanied by a deeper physical understanding and more sophisticated fabrication techniques, the NCs are now being integrated into many of the optoelectronic devices and are of prime importance for the next-generation optoelectronics. Despite all the progress, however, the full potential and synthesis dynamics of the NCs still need further investigation. Here, we addressed specifically four key aspects of the semiconductor NCs: shape engineering, electronic heterostructures, doping, and surface modification. In this thesis research, the synthesis dynamics, especially nucleation, growth and diffusion, were investigated in depth for different synthetic routes and conditions, and some of the important challenges were resolved. With the scarce number of proper emitters at longer wavelengths, in this thesis, a complex and thick heterostructure based on group II-VI nanoplatelets (NPLs) with relaxed quantum confinement was developed. The multi-shell design of the proposed NPLs helps overcome the unfavorable growth in the thickness direction, which, together with the cation dissolution/recrystallization and cation reorganization at high temperatures, relaxes the strain between the domains. The final NPLs, emitting in the deep-red region close to the bulk bandgap of CdSe, were used as an active layer in a light-emitting diode (LED) device and exhibited an exceptionally high external quantum efficiency (EQE) of 6.8% at electroluminescence peak wavelength of 701 nm, one of the best reported for colloids in this spectral range in the literature. Additionally, a novel heterostructure of multi-crown NPLs was designed and demonstrated, where several direct and indirect recombination pathways give rise to photoluminescence with both type-I and type-II characteristics. The design of these NPLs, especially the size of the domains, was shown to significantly impact the final optical properties that can activate/deactivate the recombination channels alongside the temperature. These multi-crown type-II NPLs exhibit an extremely high two-photon absorption cross-section with the highest value of 12.9 × 106 GM and low dark-bright exciton splitting energy critical for optoelectronic applications, including photodetectors, bioimaging and quantum devices. Next, we showed silver doping dynamics of core/shell NPLs, which previously proved challenging due to the self-purification after the shell growth. Here, the composition of the shell was shown to be an important factor in the destruction mechanism of the NPLs in the irreversible doping regime at high doping temperatures. The Ag:CdSe/CdZnS core/shell NPLs exhibit only dopant emission with superior paramagnetic properties compared to CdS-shelled NPLs thanks to better lattice preservation and higher dopant content. At last, a surface modification method was suggested and demonstrated for group I-III-VI NCs to enhance their electronic properties. Replacing the long-chain organic ligands with a S2- layer, injection of a negative charge and passivation of donor sites changed the behavior of the field-effect transistors (FETs) based on these NCs from p-type to n-type with more than a 105-fold enhancement in the carrier mobility. This method allowed fine-tuning of the optical properties of the NCs by the diffusion of the cations and shell formation. The findings of this thesis shine light on some of the important challenges in the field of semiconductor NCs while drawing a guideline for future research on the synthetic routes and optoelectronic properties. The thesis paves the way for future device integration of the developed NCs to fully realize their potential, while the demonstration of the more elaborated properties, including nonlinear absorption, paramagnetism and dark-bright exciton splitting, encourages further fundamental studies focusing on the physics of the semiconductor NCs.Item Open Access Color enrichment solids of spectrally pure colloidal quantum wells for wide color Span in displays(Wiley-VCH Verlag GmbH & Co. KGaA, 2022-07-18) Erdem, T.; Soran Erdem, Z.; Işık, Furkan; Shabani, Farzan; Yazici, A. F.; Mutlugün, E.; Gaponik, N.; Demir, H. V.Colloidal quantum wells (CQWs) are excellent candidates for lighting and display applications owing to their narrow emission linewidths (<30 nm). However, realizing their efficient and stable light-emitting solids remains a challenge. To address this problem, stable, efficient solids of CQWs incorporated into crystal matrices are shown. Green-emitting CdSe/CdS core/crown and red-emitting CdSe/CdS core/shell CQWs wrapped into these crystal solids are employed as proof-of-concept demonstrations of light-emitting diode (LED) integration targeting a wide color span in display backlighting. The quantum yield of the green- and red-emitting CQW-containing solids of sucrose reach ≈20% and ≈55%, respectively, while emission linewidths and peak wavelengths remain almost unaltered. Furthermore, sucrose matrix preserves ≈70% and ≈45% of the initial emission intensity of the green- and red-emitting CQWs after >60 h, respectively, which is ≈4× and ≈2× better than the drop-casted CQW films and reference (KCl) host. Color-converting LEDs of these green- and red-emitting CQWs in sucrose possess luminous efficiencies 122 and 189 lm W−1elect, respectively. With the liquid crystal display filters, this becomes 39 and 86 lm W−1elect, respectively, providing with a color gamut 25% broader than the National Television Standards Committee standard. These results prove that CQW solids enable efficient and stable color converters for display and lighting applications.Item Open Access Deep-red-emitting colloidal quantum well light-emitting diodes enabled through a complex design of core/crown/double shell heterostructure(Wiley, 2022-02-24) Shabani, Farzan; Dehghanpour Baruj, Hamed; Yurdakul, Iklim; Delikanlı, Savaş; Gheshlaghi, Negar; Işık, Furkan; Liu, B.; Altıntaş, Yemliha; Canımkurbey, Betül; Demir, Hilmi VolkanExtending the emission peak wavelength of quasi-2D colloidal quantum wells has been an important quest to fully exploit the potential of these materials, which has not been possible due to the complications arising from the partial dissolution and recrystallization during growth to date. Here, the synthetic pathway of (CdSe/CdS)@(1-4 CdS/CdZnS) (core/crown)@(colloidal atomic layer deposition shell/hot injection shell) hetero-nanoplatelets (NPLs) using multiple techniques, which together enable highly efficient emission beyond 700 nm in the deep-red region, is proposed and demonstrated. Given the challenges of using conventional hot injection procedure, a method that allows to obtain sufficiently thick and passivated NPLs as the seeds is developed. Consequently, through the final hot injection shell coating, thick NPLs with superior optical properties including a high photoluminescence quantum yield of 88% are achieved. These NPLs emitting at 701 nm exhibit a full-width-at-half-maximum of 26 nm, enabled by the successfully maintained quasi-2D shape and minimum defects of the resulting heterostructure. The deep-red light-emitting diode (LED) device fabricated with these NPLs has shown to yield a high external quantum efficiency of 6.8% at 701 nm, which is on par with other types of LEDs in this spectral range. © 2021 Wiley-VCH GmbHItem Open Access Efficient generation of emissive many-body correlations in copper-doped colloidal quantum wells(Cell Press, 2022-09-21) Yu, Junhong; Sharma, Manoj; Li, Mingjie; Liu, Baiquan; Hernández-Martínez, Pedro Ludwig; Delikanli, Savaş; Sharma, Ashma; Altintas, Yemliha; Hettiarachchi, Chathuranga; Sum, Tze Chien; Demir, Hilmi Volkan; Dang, CuongColloidal quantum wells (CQWs) provide an appealing platform to achieve emissive many-body correlations for novel optoelectronic devices, given that they act as hosts for strong carrier Coulomb interactions and present suppressed Auger recombination. However, the demonstrated high-order excitonic emission in CQWs requires ultrafast pumping with high excitation levels and can only be spectrally resolved at the single-particle level under cryogenic conditions. Here, through systematic investigation using static power-dependent emission spectroscopy and transient carrier dynamics, we show that Cu-doped CdSe CQWs exhibit continuous-wave-pumped high-order excitonic emission at room temperature with a large binding energy of ∼64 meV. We attribute this unique behavior to dopant excitons in which the ultralong lifetime and the highly localized wavefunction facilitate the formation of many-body correlations. The spectrally resolved high-order excitonic emission generated at power levels compatible with solar irradiation and electrical injection might pave the way for novel solution-processed solid-state devices. © 2022 The AuthorsItem Open Access Emerging fields of colloidal nanophotonics for quality lighting to versatile lasing(Springer Verlag, 2018) Demir, Hilmi VolkanSolution-processed semiconductor nanocrystals have attracted increasingly greater interest in optoelectronics including color conversion and enrichment in quality lighting and display backlighting. Optical properties of these colloidal nanocrystals can be conveniently controlled by tailoring their shape, composition, and size in an effort to realize high-performance light generation and lasing. We now witness the expanding deployment of semiconductor nanocrystals in consumer products being adapted by giant electronics companies. Based on the rational design and control of excitonic processes in these nanocrystals, it is possible to achieve highly efficient light-emitting diodes and optically pumped lasers. In this chapter, we introduce an emerging field of nanocrystal optoelectronics with applications from quality lighting to versatile lasing. We look into the performance limits of color conversion using colloidal nanocrystals. Here we introduce a new concept of all-colloidal lasers developed by incorporating nanocrystal emitters as the optical gain media intimately into fully colloidal cavities. As an extreme case of solution-processed tightly-confined quasi-2D colloids, we also show that the atomically flat nanoplatelets uniquely offer record high optical gain coefficients and ultralow threshold stimulated emission. Given the recent accelerating progress in colloidal nanophotonics, solution-processed quantum materials now hold great promise to challenge their conventional epitaxial counterparts in the near future.Item Unknown Giant modal gain coefficients in colloidal II–VI nanoplatelets(American Chemical Society, 2019) Güzeltürk, Burak; Pelton, M.; Olutaş, Murat; Demir, Hilmi VolkanModal gain coefficient is a key figure of merit for a laser material. Previously, net modal gain coefficients larger than a few thousand cm–1 were achieved in II–VI and III–V semiconductor gain media, but this required operation at cryogenic temperatures. In this work, using pump-fluence-dependent variable-stripe-length measurements, we show that colloidal CdSe nanoplatelets enable giant modal gain coefficients at room temperature up to 6600 cm–1 under pulsed optical excitation. Furthermore, we show that exceptional gain performance is common to the family of CdSe nanoplatelets, as shown by examining samples having different vertical thicknesses and lateral areas. Overall, colloidal II–VI nanoplatelets with superior optical gain properties are promising for a broad range of applications, including high-speed light amplification and loss compensation in plasmonic photonic circuits.Item Open Access Gradient Type-II CdSe/CdSeTe/CdTe Core/Crown/Crown heteronanoplatelets with asymmetric shape and disproportional excitonic properties(Wiley-VCH Verlag GmbH & Co. KGaA, 2023-01-17) Shabani, Farzan; Hernandez Martinez, P. L.; Shermet, Nina; Korkut, Hilal; Sarpkaya, İbrahim; Baruj, Hamed Dehghanpour; Delikanlı, Savaş; Işık, Furkan; Durmuşoğlu, E. G.; Demir, Hilmi VolkanCharacterized by their strong 1D confinement and long-lifetime red-shifted emission spectra, colloidal nanoplatelets (NPLs) with type-II electronic structure provide an exciting ground to design complex heterostructures with remarkable properties. This work demonstrates the synthesis and optical characterization of CdSe/CdSeTe/CdTe core/crown/crown NPLs having a step-wise gradient electronic structure and disproportional wavefunction distribution, in which the excitonic properties of the electron and hole can be finely tuned through adjusting the geometry of the intermediate crown. The first crown with staggered configuration gives rise to a series of direct and indirect transition channels that activation/deactivation of each channel is possible through wavefunction engineering. Moreover, these NPLs allow for switching between active channels with temperature, where lattice contraction directly affects the electron–hole (e–h) overlap. Dominated by the indirect transition channels over direct transitions, the lifetime of the NPLs starts to increase at 9 K, indicative of low dark-bright exciton splitting energy. The charge transfer states from the two type-II interfaces promote a large number of indirect transitions, which effectively increase the absorption of low-energy photons critical for nonlinear properties. As a result, these NPLs demonstrate exceptionally high two-photon absorption cross-sections with the highest value of 12.9 × 10$^{6}$ GM and superlinear behavior.Item Open Access High external quantum efficiency light-emitting diodes enabled by advanced heterostructures of type-ii nanoplatelets(American Chemical Society, 2023-03-13) Durmusoglu, Emek G.; Hu, Sujuan; Hernandez-Martinez, Pedro Ludwig; Izmir, Merve; Shabani,Farzan; Guo, Min; Gao, Huayu; Isik, Furkan; Delikanli, Savas; Sharma, Vijay Kumar; Liu, Baiquan; Demir, Hilmi VolkanColloidal quantum wells (CQWs), also known as nanoplatelets (NPLs), are exciting material systems for numerous photonic applications, including lasers and light-emitting diodes (LEDs). Although many successful type-I NPL-LEDs with high device performance have been demonstrated, type-II NPLs are not fully exploited for LED applications, even with alloyed type-II NPLs with enhanced optical properties. Here, we present the development of CdSe/CdTe/CdSe core/crown/crown (multi-crowned) type-II NPLs and systematic investigation of their optical properties, including their comparison with the traditional core/crown counterparts. Unlike traditional type-II NPLs such as CdSe/CdTe, CdTe/CdSe, and CdSe/CdSexTe1–x core/crown heterostructures, here the proposed advanced heterostructure reaps the benefits of having two type-II transition channels, resulting in a high quantum yield (QY) of 83% and a long fluorescence lifetime of 73.3 ns. These type-II transitions were confirmed experimentally by optical measurements and theoretically using electron and hole wave function modeling. Computational study shows that the multi-crowned NPLs provide a better-distributed hole wave function along the CdTe crown, while the electron wave function is delocalized in the CdSe core and CdSe crown layers. As a proof-of-concept demonstration, NPL-LEDs based on these multi-crowned NPLs were designed and fabricated with a record high external quantum efficiency (EQE) of 7.83% among type-II NPL-LEDs. These findings are expected to induce advanced designs of NPL heterostructures to reach a fascinating level of performance, especially in LEDs and lasers.Item Open Access High external quantum efficiency light-emitting diodes enabled by advanced heterostructures of Type-II nanoplatelets(American Chemical Society, 2023-04-25) Durmuşoğlu, E. G.; Hu, S.; Hernandez-Martinez, P. L.; İzmir, M.; Shabani, Farzan; Guo, M.; Gao, H.; Işık, Furkan; Delikanlı, Savaş; Sharma, V. K.; Liu, B.; Demir, Hilmi VolkanColloidal quantum wells (CQWs), also known as nanoplatelets (NPLs), are exciting material systems for numerous photonic applications, including lasers and light-emitting diodes (LEDs). Although many successful type-I NPL-LEDs with high device performance have been demonstrated, type-II NPLs are not fully exploited for LED applications, even with alloyed type-II NPLs with enhanced optical properties. Here, we present the development of CdSe/CdTe/CdSe core/crown/crown (multi-crowned) type-II NPLs and systematic investigation of their optical properties, including their comparison with the traditional core/crown counterparts. Unlike traditional type-II NPLs such as CdSe/CdTe, CdTe/CdSe, and CdSe/CdSexTe1–x core/crown heterostructures, here the proposed advanced heterostructure reaps the benefits of having two type-II transition channels, resulting in a high quantum yield (QY) of 83% and a long fluorescence lifetime of 73.3 ns. These type-II transitions were confirmed experimentally by optical measurements and theoretically using electron and hole wave function modeling. Computational study shows that the multi-crowned NPLs provide a better-distributed hole wave function along the CdTe crown, while the electron wave function is delocalized in the CdSe core and CdSe crown layers. As a proof-of-concept demonstration, NPL-LEDs based on these multi-crowned NPLs were designed and fabricated with a record high external quantum efficiency (EQE) of 7.83% among type-II NPL-LEDs. These findings are expected to induce advanced designs of NPL heterostructures to reach a fascinating level of performance, especially in LEDs and lasers.Item Open Access High-efficiency optical gain in type-II semiconductor nanocrystals of alloyed colloidal quantum wells(American Chemical Society, 2017) Guzelturk, B.; Kelestemur Y.; Olutas M.; Li, Q.; Lian, T.; Demir, Hilmi VolkanColloidal nanocrystals having controlled size, tailored shape, and tuned composition have been explored for optical gain and lasing. Among these, nanocrystals having Type-II electronic structure have been introduced toward low-threshold gain. However, to date, their performance has remained severely limited due to diminishing oscillator strength and modest absorption cross-section. Overcoming these problems, here we realize highly efficient optical gain in Type-II nanocrystals by using alloyed colloidal quantum wells. With composition-tuned core/alloyed-crown CdSe/CdSexTe1-x quantum wells, we achieved amplified spontaneous emission thresholds as low as 26 μJ/cm2, long optical gain lifetimes (τgain ≈ 400 ps), and high modal gain coefficients (gmodal ≈ 930 cm-1). We uncover that the optical gain in these Type-II quantum wells arises from the excitations localized to the alloyed-crown region that are electronically coupled to the charge-transfer state. These alloyed heteronanostructures exhibiting remarkable optical gain performance are expected to be highly appealing for future display and lighting technologies.Item Open Access Lateral size-dependent spontaneous and stimulated emission properties in colloidal CdSe nanoplatelets(American Chemical Society, 2015) Olutaş, M.; Güzeltürk, B.; Keleştemur, Y.; Yeltik A.; Delikanlı, S.; Demir, Hilmi VolkanHere, we systematically investigated the spontaneous and stimulated emission performances of solution-processed atomically flat quasi-2D nanoplatelets (NPLs) as a function of their lateral size using colloidal CdSe core NPLs. We found that the photoluminescence quantum efficiency of these NPLs decreases with increasing lateral size while their photoluminescence decay rate accelerates. This strongly suggests that nonradiative channels prevail in the NPL ensembles having extended lateral size, which is well-explained by the increasing number of the defected NPL subpopulation. In the case of stimulated emission the role of lateral size in NPLs influentially emerges both in the single- and two-photon absorption (1PA and 2PA) pumping. In the amplified spontaneous emission measurements, we uncovered that the stimulated emission thresholds of 1PA and 2PA exhibit completely opposite behavior with increasing lateral size. The NPLs with larger lateral sizes exhibited higher stimulated emission thresholds under 1PA pumping due to the dominating defected subpopulation in larger NPLs. On the other hand, surprisingly, larger NPLs remarkably revealed lower 2PA-pumped amplified spontaneous emission thresholds. This is attributed to the observation of a "giant" 2PA cross-section overwhelmingly growing with increasing lateral size and reaching record levels higher than 10(6) GM, at least an order of magnitude stronger than colloidal quantum dots and rods. These findings suggest that the lateral size control in the NPLs, which is commonly neglected, is essential to high-performance colloidal NPL optoelectronic devices in addition to the vertical monolayer control.Item Open Access Light-Emitting diodes with Cu-Doped colloidal quantum wells: from ultrapure green, tunable dual-emission to white light(WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim, 2019) Liu, B.; Sharma, Manoj; Yu, J.; Shendre, S.; Hettiarachchi, C.; Sharma, Ashma; Yeltik, Aydan; Wang, L.; Sun, H.; Dang, C.; Demir, Hilmi VolkanCopper‐doped colloidal quantum wells (Cu‐CQWs) are considered a new class of optoelectronic materials. To date, the electroluminescence (EL) property of Cu‐CQWs has not been revealed. Additionally, it is desirable to achieve ultrapure green, tunable dual‐emission and white light to satisfy the various requirement of display and lighting applications. Herein, light‐emitting diodes (LEDs) based on colloidal Cu‐CQWs are demonstrated. For the 0% Cu‐doped concentration, the LED exhibits Commission Internationale de L'Eclairage 1931 coordinates of (0.103, 0.797) with a narrow EL full‐wavelength at half‐maximum of 12 nm. For the 0.5% Cu‐doped concentration, a dual‐emission LED is realized. Remarkably, the dual emission can be tuned by manipulating the device engineering. Furthermore, at a high doping concentration of 2.4%, a white LED based on CQWs is developed. With the management of doping concentrations, the color tuning (green, dual‐emission to white) is shown. The findings not only show that LEDs with CQWs can exhibit polychromatic emission but also unlock a new direction to develop LEDs by exploiting 2D impurity‐doped CQWs that can be further extended to the application of other impurities (e.g., Mn, Ag).Item Open Access Low-threshold lasing from copper-doped CdSe colloidal quantum wells(Wiley, 2021-05-04) Yu, J.; Sharma, M.; Li, M.; Delikanlı, Savaş; Sharma, A.; Taimoor, M.; Altintas, Y.; McBride, J. R.; Kusserow, T.; Sum, T.; Demir, Hilmi VolkanTransition metal doped colloidal nanomaterials (TMDCNMs) have recently attracted attention as promising nano-emitters due to dopant-induced properties. However, despite ample investigations on the steady-state and dynamic spectroscopy of TMDCNMs, experimental understandings of their performance in stimulated emission regimes are still elusive. Here, the optical gain properties of copper-doped CdSe colloidal quantum wells (CQWs) are systemically studied with a wide range of dopant concentration for the first time. This work demonstrates that the amplified spontaneous emission (ASE) threshold in copper-doped CQWs is a competing result between the biexciton formation, which is preferred to achieve population inversion, and the hole trapping which stymies the population inversion. An optimum amount of copper dopants enables the lowest ASE threshold of ≈7 µJ cm−2, about 8-fold reduction from that in undoped CQWs (≈58 µJ cm−2) under sub-nanosecond pulse excitation. Finally, a copper-doped CQW film embedded in a vertical cavity surface-emitting laser (VCSEL) structure yields an ultralow lasing threshold of 4.1 µJ cm−2. Exploiting optical gain from TMDCNMs may help to further boost the performance of colloidal-based lasers.Item Open Access Low-threshold optical gain and lasing of colloidal nanoplatelets(IEEE, 2014-10) Keleştemur, Yusuf; Güzeltürk, Burak; Olutaş, Murat; Delikanlı, Savaş; Demir, Hilmi VolkanSemiconductor nanocrystals, which are also known as colloidal quantum dots (CQDs), are highly attractive materials for high performance optoelectronic device applications such as lasers. With their size, shape and composition tunable electronic structure and optical properties, CQDs are highly desired for achieving full-color, temperature-insensitive, low-threshold and solution-processed lasers [1, 2]. However, due to their small size, they suffer from the nonradiative multiexciton Auger Recombination (AR), where energy of a bound electron-hole pair is transferred to a third particle of either an electron or a hole instead of radiative recombination. Therefore, CQDs having suppressed AR are strongly required for achieving high quality CQD-based lasers. To address this issue, CQDs having different size, shape and electronic structure have been synthesized and studied extensively [3-5]. Generally, suppression of AR and lower optical gain thresholds are achieved via reducing the wavefunction overlap of the electron and hole in a CQD. However, the separation of the electron and hole wavefunctions will dramatically decrease the oscillator strength and optical gain coefficient, which is highly critical for achieving high performance lasers. Therefore, colloidal materials with suppressed AR and high gain coefficients are highly welcomed. Here, we study optical gain performance of colloidal quantum wells [6] of CdSe-core and CdSe/CdS core/crown nanoplatelets (NPLs) that demonstrate remarkable optical properties with ultra-low threshold one- and two-photon optical pumping. As a result of their giant oscillator strength, superior optical gain and lasing performance are achieved from these colloidal NPLs with greatly enhanced gain coefficient [7]. © 2014 IEEE.Item Open Access Modulating emission properties in a host–guest colloidal quantum well superlattice(Wiley-VCH Verlag GmbH & Co. KGaA, 2021-12-19) Yu, J.; Sharma, Manoj; Wang, Y.; Delikanlı, S.; Baruj, Hamed Dehghanpour; Sharma, A.; Demir, Hilmi VolkanSelf-assembly of colloidal nanocrystals into ordered superlattices is a powerful approach to enable novel collective properties which are not available in individual colloids. However, to date, it remains a major challenge to develop a practical route to modulate such collective properties for potential photonic applications. Herein, it is shown that the collective emission properties in colloidal quantum well (CQW) superlattices, including emission color and anisotropy, can be effectively modulated in a binary host–guest architecture. The experimental and theoretical results reveal that excitons of the host (i.e., the undoped CQWs) generated by photoexcitation can be controllably harvested by the guest (i.e., the Cu-doped CQWs) for light emission, owing to an exciton hopping assisted exciton trapping process. Such a nano-building block with tunable collective optical properties may enlighten novel colloidal material-based photonic applications, including optical anti-counterfeiting, next-generation liquid crystal displays, and multifunctional biological markers.Item Open Access Near-Infrared-Emitting five-monolayer thick copper-doped CdSe nanoplatelets(WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim, 2019) Sharma, Ashma; Sharma, Manoj; Güngör, Kıvanç; Olutaş, Murat; Dede, Didem; Demir, Hilmi VolkanDoped nanocrystals are instrumental to the high‐performance luminescent solar concentrators (LSCs) and the color conversion devices. Recently, copper (Cu)‐doped three and four monolayer (ML) thick CdSe nanoplatelets (NPLs) have been shown superior to the existing Cu‐doped quantum dots (QDs) for their use in LSCs. However, additional improvement in the LSC performance can be achieved by further redshifting the emission into the near‐infrared (NIR) region of electromagnetic spectrum and increasing the absorbed portion of the solar irradiation. Cu‐doping into higher thicknesses of these atomically flat NPLs (e.g., ≥5 ML) can achieve these overarching goals. However, addition of the dopant ions during the nucleation stage disturbs this high‐temperature growth process and leads to multiple populations of NPLs and QDs. Here, by carefully controlling the precursor chemistry the successful doping of Cu in five ML thick NPLs by high‐temperature nucleation doping method is demonstrated. The optimized synthesis method shows nearly pure population of doped five ML thick NPLs, which possess ≈150 nm Stokes‐shifted NIR emission with high quantum yield of 65 ± 2%. Structural, elemental, and optical studies are conducted to confirm the successful doping and understand the detailed photophysics. Finally, these materials are tested experimentally and theoretically for their performance as promising LSC materials.Item Open Access Near-unity emitting copper-doped colloidal semiconductor quantum wells for luminescent solar concentrators(Wiley-VCH Verlag, 2017) Sharma, M.; Gungor K.; Yeltik A.; Olutas M.; Guzelturk, B.; Kelestemur Y.; Erdem, T.; Delikanli S.; McBride, J. R.; Demir, Hilmi VolkanDoping of bulk semiconductors has revealed widespread success in optoelectronic applications. In the past few decades, substantial effort has been engaged for doping at the nanoscale. Recently, doped colloidal quantum dots (CQDs) have been demonstrated to be promising materials for luminescent solar concentrators (LSCs) as they can be engineered for providing highly tunable and Stokes-shifted emission in the solar spectrum. However, existing doped CQDs that are aimed for full solar spectrum LSCs suffer from moderately low quantum efficiency, intrinsically small absorption cross-section, and gradually increasing absorption profiles coinciding with the emission spectrum, which together fundamentally limit their effective usage. Here, the authors show the first account of copper doping into atomically flat colloidal quantum wells (CQWs). In addition to Stokes-shifted and tunable dopant-induced photoluminescence emission, the copper doping into CQWs enables near-unity quantum efficiencies (up to ≈97%), accompanied by substantially high absorption cross-section and inherently step-like absorption profile, compared to those of the doped CQDs. Based on these exceptional properties, the authors have demonstrated by both experimental analysis and numerical modeling that these newly synthesized doped CQWs are excellent candidates for LSCs. These findings may open new directions for deployment of doped CQWs in LSCs for advanced solar light harvesting technologies.