Browsing by Subject "Colloidal nanoplatelets"

Now showing 1 - 14 of 14

Open Access
Amplified Spontaneous Emission and Lasing in Colloidal Nanoplatelets
(American Chemical Society, 2014-07) Guzelturk, B.; Kelestemur, Y.; Olutas, M.; Delikanli, S.; Demir, Hilmi Volkan
Colloidal nanoplatelets (NPLs) have recently emerged as favorable light-emitting materials, which also show great potential as optical gain media due to their remarkable optical properties. In this work, we systematically investigate the optical gain performance of CdSe core and CdSe/CdS core/crown NPLs having different CdS crown size with one- and two-photon absorption pumping. The core/crown NPLs exhibit enhanced gain performance as compared to the core-only NPLs due to increased absorption cross section and the efficient interexciton funneling, which is from the CdS crown to the CdSe core. One- and two-photon absorption pumped amplified spontaneous emission thresholds are found as low as 41 μJ/cm2 and 4.48 mJ/cm2 , respectively. These thresholds surpass the best reported optical gain performance of the state-of-the-art colloidal nanocrystals (i.e., quantum dots, nanorods,etc.) emitting in the same spectral range as the NPLs. Moreover, gain coefficient of the NPLs is measured as high as 650 cm 1 , which is 4-fold larger than the best reported gain coefficient of the colloidal quantum dots. Finally, we demonstrate a two-photon absorption pumped vertical cavity surface emitting laser of the NPLs with a lasing threshold as low as 2.49 mJ/cm2 . These excellent results are attributed to the superior properties of the NPLs as optical gain media.
Open Access
Blue-emitting CdSe nanoplatelets enabled by sulfur-alloyed heterostructures for light-emitting diodes with low turn-on voltage
(American Chemical Society, 2021-12-28) İzmir, M.; Sharma, A.; Shendre, S.; Durmuşoğlu, E. G.; Sharma, V. K.; Shabani, Farzan; Baruj, Hamed Dehghanpour; Delikanlı, Savaş; Sharma, M.; Demir, Hilmi Volkan
Colloidal nanoplatelets (NPLs) have emerged as the last class of semiconductor nanocrystals for their potential optoelectronic applications. The heterostructures of these nanocrystals can achieve high photoluminescence quantum yield and enhanced photostability, along with color purity. Such advantages make them a promising candidate for solution-processable light-emitting diodes (LEDs). However, to date, blue-emitting CdSe nanoplatelets (NPLs) exhibit poor photoluminescence quantum yield and also typically suffer from a rolled-up morphology. To mitigate these problems in this work, we propose and demonstrate efficient alloyed 4 ML CdSe1–xSx nanoplatelets having a CdS crown with enhanced photoluminescence quantum yields (up to 60%) in the blue region (462–487 nm). We successfully used these NPLs as an electrically driven active emitter in the blue-emitting NPL-LEDs with a low turn-on voltage of ∼4 V. The Commission Internationale de L’Eclairage (CIE) coordinates of (0.23, 0.14) were obtained for these blue-emitting NPL-LEDs. These emitters could potentially open up the opportunity for full-color displays using these NPL-based blue LEDs in conjunction with the red and green ones.
Open Access
Colloidal doping of thick nanoplatelets
(2022-12) Ahmad, Muhammad
Semiconductor nanoplatelets (NPLs) make an interesting group of nanocrystals with unique optical properties as a result of their quasi 2-dimensional (2D) electronic structure. Such emerging fascinating optical features of NPLs include high absorption cross-section, narrow emission linewidths, and reduced Auger recombination, making them a superior choice compared to conventional semiconductor nanocrystals for optoelectronic applications. Doping of these materials with transition metals, such as silver and copper, provides great opportunities to modify and tune the electronic structure of these NPLs for various devices including light-emitting diodes and luminescent solar concentrators. Such doping with transition metals allows for manipulation of the photoluminescence from these NPLs, control of the recombination processes of the photogenerated carriers in these NPLs, and observation of the giant Zeeman effect as a result of exchange interactions between the dopants and carriers in these NPLs. Previously, CdSe NPLs have been doped with copper and silver only up to vertical thickness of 5 monolayers (ML). However, doping of thicker NPLs has not been possible to date. In this thesis work, we successfully doped thick CdSe NPLs having 7 ML in thickness with silver and copper using partial cation exchange to obtain large Stokes-shifted emission in the near-infrared (NIR) region. Here, the effect of precursor ratio and reaction temperature were systematically studied to tune the resulting emission. For both copper and silver dopants, we successfully quenched fully the band-edge emission, and purely dopantinduced emission was obtained. We also co-doped these NPLs with silver and copper, and we successfully obtained both copper- and silver-induced emissions from these NPLs. We further grew the CdZnS shell on 7 ML CdSe core by hot injection method and doped the resulting CdSe/CdZnS core/shell NPLs with silver and copper to push their emission further towards longer wavelengths in the NIR region. These thick doped-NPLs with large Stokes shift and emission in the NIR region present a promising platform for light-emitting and -harvesting applications.
Open Access
Colloidal heterostructures of semiconductor quantum wells : synthesis, characterization and applications
(2017-06) Keleştemur, Yusuf
Colloidal semiconductor quantum wells, also known as nanoplatelets (NPLs), have recently emerged as a new class of colloidal semiconductor nanocrystals enabling fascinating excitonic properties. With their quasi two-dimensional structure resembling epitaxially-grown quantum wells, these atomically- at nanoplatelets exhibit narrow emission linewidths, giant linear and nonlinear absorption cross-sections, and ultrafast uorescence lifetimes when compared to other classes of semiconductor nanocrystals. These appealing features have led to achievement of low lasing thresholds and high color purity by using simple heterostructures of these NPLs. To further exploit the benefits of these solutionprocessed NPLs and develop next-generation colloidal optoelectronic devices, novel heterostructures of NPLs with superior excitonic properties are in high demand. In this thesis, to address these needs, we proposed and demonstrated novel heterostructured NPLs. This thesis includes the rational design and systematic synthesis and characterization of these hetero-NPLs. To overcome the lower photoluminescence quantum yield (PL-QY) and stability issues of core/shell NPLs, we successfully synthesized CdSe/CdS/CdS core/crown/shell NPLs resembling platelet-in-a-box. With this advanced architecture, we accomplished substantially enhanced PL-QY and absorption crosssection as well as stability, allowing for the achievement of low-threshold optical gain. However, due to the pure vertical confinement observed in these NPLs, these exciting excitonic features of NPLs suffered from the limited spectral tunability. By developing homogenously alloyed CdSexS1 NPLs together with their alloyed core/crown and alloyed core/shell heterostructures, we succeeded in obtaining highly tunable excitonic features and further extending tunability of the optical gain from these NPLs. In addition to the NPLs having Type-I electronic structure, we demonstrated the highly uniform growth of CdSe/CdTe core/crown NPLs having Type-II electronic structure exhibiting unique excitonic properties Additionally, to realize the evolution of Type-II electronic structure, we synthesized CdSe/CdSe1-xTex core/crown NPLs by precisely tailoring the composition of the crown region. Without changing their vertical thicknesses, we achieved again highly tunable excitonic features and near-unity PL-QY from these hetero- NPLs. Based on the proposed architectures of these heteronanoplatelets, we believe the findings of this thesis provide important guidelines and inspiration for the synthesis of highly efficient and stable heterostructured NPLs to construct high-performance colloidal optoelectronic devices, possibly challenging their conventional epitaxially-grown counterparts.
Open Access
Colloidal nanoplatelets-based soft matter technology for photonic interconnected networks: low-threshold lasing and polygonal self-coupling microlasers
(Wiley-VCH GmbH, 2023-11-15) Duan, Rui; Thung, Yi Tian; Zhang, Zitong; Durmuşoğlu, Emek Göksu; He, Yichen; Xiao, Lian; Lee, Calvin Xiu Xian; Lew, Wen Siang; Zhang, Lin; Li, Hanyang; Yang, Jun; Demir, Hilmi Volkan; Sun, Handong
Soft matter-based microlasers are widely regarded as excellent building blocks for realizing photonic interconnected networks in optoelectronic chips, owing to their flexibility and functional network topology. However, the potential of these devices is hindered by challenges such as poor lasing stability, high lasing threshold, and gaps in knowledge regarding cavity interconnection characteristics. In this study, the first demonstration of a high-quality, low-threshold nanoplatelets (NPLs)-based polymer microfiber laser fabricated using capillary immersion techniques and its photonic interconnected networks are presented. CdSe/CdS@Cd1-xZnxS core/buffer shell@graded-shell NPLs with high optical gain characteristics are adopted as the gain medium. The study achieves a lasing threshold below 14.8 mu J cm-2, a single-mode quality (Q)-factor of approximate to 5500, and robust lasing stability in the fabricated NPLs-based microfibers. Furthermore, the study pioneers the exploration of polygonal self-coupling microlasers and the optical characteristics of their interconnected fiber network. Based on the signal generation mechanism observed in the photonic networks, an interconnected NPLs-based fiber network structure achieving single-mode lasing emission and laser mode modulation is successfully designed. The work contributes a novel method for realizing microlasers fabricated via soft-matter technologies and provides a key foundation and new insights for unit design and programming for future photonic network systems.
Open Access
Colloidal synthesis of Ag(I)-doped CdSe nanoplatelets with partial cation exchange method
(2019-01) Bozdoğan, İrfan Selim
Colloidal nanoplatelets (NPLs) exhibit strong one-dimensional quantum confinement in the vertical direction. This makes them a highly attractive host system for studying variable doping techniques and effects without variation in the quantum confinement effect. Earlier, core-only CdSe NPLs were converted into Cu2Se and HgSe NPLs, and also CdSe/CdS core/shell NPLs were transformed into Cu2Se/Cu2S, ZnSe/ZnS, and PbSe/PbS NPLs by using full cation exchange (CE) methods. Recently, core-only CdSe NPLs have been doped with Cu(I) ions using high-temperature nucleation doping and post-synthesis partial CE approaches. On the other hand, unlike Cu(I), such monovalent doping with Ag(I) ions has previously not been possible in NPLs as a host system, although silver doping had been widely studied in other host systems. Therefore, there has been no previous report on the doping of Ag(I) into CdSe NPLs to date. To address this gap, in this thesis, Ag(I) doping in CdSe NPLs by using a postsynthesis partial CE technique was developed. A systematic study was carried out to investigate the effects of dopant precursor reactivities, reaction timing, and temperature on the evolution of dopant-related emission as compared to the excitonic emission. In controlled experiments, the excitonic emission peak was eliminated and only dopant-related emission peak was successfully obtained. Finally, temperaturedependent emission kinetics of the as-synthesized Ag(I)-doped CdSe NPLs at varied temperatures ranging from 25 to 298 K were investigated. It was observed that both excitonic and dopant-related emission peaks were blue-shifted and their intensities were considerably increased with the decreasing temperature. As a new dopant-host system, these Ag(I)-doped CdSe NPLs hold a great promise for further systematic spectroscopic studies and possibly various optoelectronic applications.
Open Access
Continuously tunable emission in inverted type ‐ I CdS/CdSe core/crown semiconductor nanoplatelets
(Wiley, 2015-07-15) Delikanlı, S.; Güzeltürk, B.; Hernandez - Martinez, P. L.; Erdem, T.; Keleştemur, Y.; Olutas M.; Akgül, M. Z.; Demir, Hilmi Volkan
The synthesis and unique tunable optical properties of core/crown nanoplatelets having an inverted Type-I heterostructure are presented. Here, colloidal 2D CdS/CdSe heteronanoplatelets are grown with thickness of four monolayers using seed-mediated method. In this work, it is shown that the emission peak of the resulting CdS/CdSe heteronanoplatelets can be continuously spectrally tuned between the peak emission wavelengths of the core only CdS nanoplatelets (421 nm) and CdSe nanoplatelets (515 nm) having the same vertical thickness. In these inverted Type-I nanoplatelets, the unique continuous tunable emission is enabled by adjusting the lateral width of the CdSe crown, having a narrower bandgap, around the core CdS nanoplatelet, having a wider bandgap, as a result of the controlled lateral quantum confinement in the crown region additional to the pure vertical confinement. As a proof-of-concept demonstration, a white light generation is shown by using color conversion with these CdS/CdSe heteronanoplatelets having finely tuned thin crowns, resulting in a color rendering index of 80. The robust control of the electronic structure in such inverted Type-I heteronanoplatelets achieved by tailoring the lateral extent of the crown coating around the core template presents a new enabling pathway for bandgap engineering in solution-processed quantum wells.
Open Access
Giant modal gain coefficients in colloidal II–VI nanoplatelets
(American Chemical Society, 2019) Güzeltürk, Burak; Pelton, M.; Olutaş, Murat; Demir, Hilmi Volkan
Modal 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.
Open Access
Near-field energy transfer into silicon inversely proportional to distance using quasi-2D colloidal quantum well donors
(Wiley-VCH Verlag GmbH & Co. KGaA, 2021-09-12) Humayun, Muhammad Hamza; Hernandez-Martinez, Pedro Ludwig; Gheshlaghi, Negar; Erdem, Onur; Altıntaş, Yemliha; Shabani, Farzan; Demir, Hilmi Volkan
Silicon is the most prevalent material system for light-harvesting applications; however, its inherent indirect bandgap and consequent weak absorption limits its potential in optoelectronics. This paper proposes to address this limitation by combining the sensitization of silicon with extraordinarily large absorption cross sections of quasi-2D colloidal quantum well nanoplatelets (NPLs) and to demonstrate excitation transfer from these NPLs to bulk silicon. Here, the distance dependency, d, of the resulting Förster resonant energy transfer from the NPL monolayer into a silicon substrate is systematically studied by tuning the thickness of a spacer layer (of Al2O3) in between them (varied from 1 to 50 nm in thickness). A slowly varying distance dependence of d−1 with 25% efficiency at a donor–acceptor distance of 20 nm is observed. These results are corroborated with full electromagnetic solutions, which show that the inverse distance relationship emanates from the delocalized electric field intensity across both the NPL layer and the silicon because of the excitation of strong in-plane dipoles in the NPL monolayer. These findings pave the way for using colloidal NPLs as strong light-harvesting donors in combination with crystalline silicon as an acceptor medium for application in photovoltaic devices and other optoelectronic platforms.
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 Volkan
A 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.
Open Access
Optical gain and lasing of colloidal semiconductor quantum wells intimately integrated into optical cavities
(2019-07) Sak, Mustafa
Colloidal semiconductor quantum wells, also known as nanoplatelets (NPLs), attract an increasingly greater deal of interest as a promising material platform for light-generating applications. The superior optical properties of NPLs including their ultra-large absorption cross-sections, purely homogeneous broadening, and suppressed Auger recombination make them highly attractive for solution-processable color convertors, LEDs and lasers. In this thesis, we studied the optical gain properties and performance levels of tailored heterostructures of such NPLs intimately integrated into various optical cavities. To do so, we systematically measured their amplified spontaneous emission under one- and twophoton absorption excitations. Also, with these hetero-NPLs as the gain media, we have proposed and demonstrated a new class of practical whispering gallery mode (WGM) NPL-fiber architecture with high stability and low lasing thresholds enabled by record low waveguide loss coefficients in its class. Moreover, we have developed a single-mode vertical-cavity surface-emitting laser (VCSEL) of these hetero-NPLs closely integrated into the wedge cavity of a pair of distributed Bragg reflectors, leading to a record low lasing threshold in its class. The findings obtained in these WGM NPL-laser and NPLVCSEL structures indicate that these NPLs are excellent for high-performance colloidal lasing.
Open Access
Room-temperature lasing in colloidal nanoplatelets via mie-resonant bound states in the continuum
(American Chemical Society, 2020) Wu, M.; Ha, S. T.; Shendre, S.; Durmuşoğlu, E. G.; Koh, W.-K.; Abujetas, D. R.; Sanchez-Gil, J. A.; Paniagua-Domínguez, R.; Demir, Hilmi Volkan; Kuznetsov, A. I.
Solid-state room-temperature lasing with tunability in a wide range of wavelengths is desirable for many applications. To achieve this, besides an efficient gain material with a tunable emission wavelength, a high quality-factor optical cavity is essential. Here, we combine a film of colloidal CdSe/CdZnS core–shell nanoplatelets with square arrays of nanocylinders made of titanium dioxide to achieve optically pumped lasing at visible wavelengths and room temperature. The all-dielectric arrays support bound states in the continuum (BICs), which result from lattice-mediated Mie resonances and boast infinite quality factors in theory. In particular, we demonstrate lasing from a BIC that originates from out-of-plane magnetic dipoles oscillating in phase. By adjusting the diameter of the cylinders, we tune the lasing wavelength across the gain bandwidth of the nanoplatelets. The spectral tunability of both the cavity resonance and nanoplatelet gain, together with efficient light confinement in BICs, promises low-threshold lasing with wide selectivity in wavelengths.
Open Access
Stacking in colloidal nanoplatelets: tuning excitonic properties
(American Chemical Society, 2014) Guzelturk, B.; Erdem, O.; Olutas M.; Kelestemur Y.; Demir, Hilmi Volkan
Colloidal semiconductor quantum wells, also commonly known as nanoplatelets (NPLs), have arisen among the most promising materials for light generation and harvesting applications. Recently, NPLs have been found to assemble in stacks. However, their emerging characteristics essential to these applications have not been previously controlled or understood. In this report, we systematically investigate and present excitonic properties of controlled column-like NPL assemblies. Here, by a controlled gradual process, we show that stacking in colloidal quantum wells substantially increases exciton transfer and trapping. As NPLs form into stacks, surprisingly we find an order of magnitude decrease in their photoluminescence quantum yield, while the transient fluorescence decay is considerably accelerated. These observations are corroborated by ultraefficient Forster resonance energy transfer (FRET) in the stacked NPLs, in which exciton migration is estimated to be in the ultralong range (>100 nm). Homo-FRET (i.e., FRET among the same emitters) is found to be ultraefficient, reaching levels as high as 99.9% at room temperature owing to the close-packed collinear orientation of the NPLs along with their large extinction coefficient and small Stokes shift, resulting in a large Forster radius of similar to 13.5 nm. Consequently, the strong and long-range homo-FRET boosts exciton trapping in nonemissive NPLs, acting as exciton sink centers, quenching photoluminescence from the stacked NPLs due to rapid nonradiative recombination of the trapped excitons. The rate-equation-based model, which considers the exciton transfer and the radiative and nonradiative recombination within the stacks, shows an excellent match with the experimental data. These results show the critical significance of stacking control in NPL solids, which exhibit completely different signatures of homo-FRET as compared to that in colloidal nanocrystals due to the absence of inhomogeneous broadening.
Open Access
Thickness-tunable self-assembled colloidal nanoplatelet films enable ultrathin optical gain media
(American Chemical Society, 2020) Erdem, Onur; Foroutan, Sina; Gheshlaghi, Negar; Güzeltürk, B.; Altıntaş, Yemliha; Demir, Hilmi Volkan
We propose and demonstrate construction of highly uniform, multilayered superstructures of CdSe/CdZnS core/shell colloidal nanoplatelets (NPLs) using liquid interface self-assembly. These NPLs are sequentially deposited onto a solid substrate into slabs having monolayer-precise thickness across tens of cm2 areas. Because of near-unity surface coverage and excellent uniformity, amplified spontaneous emission (ASE) is observed from an uncharacteristically thin film having 6 NPL layers, corresponding to a mere 42 nm thickness. Furthermore, systematic studies on optical gain of these NPL superstructures having thicknesses ranging from 6 to 15 layers revealed the gradual reduction in gain threshold with increasing number of layers, along with a continuous spectral shift of the ASE peak (∼18 nm). These observations can be explained by the change in the optical mode confinement factor with the NPL waveguide thickness and propagation wavelength. This bottom-up construction technique for thickness-tunable, three-dimensional NPL superstructures can be used for large-area device fabrication.