Browsing by Subject "Semiconductor Nanocrystals"

Now showing 1 - 10 of 10

Open Access
Attractive versus repulsive excitonic interactions of colloidal quantum dots control blue-to red-shifting (and non-shifting) amplified spontaneous emission
(American Chemical Society, 2013-11-21) Cihan, A. F.; Kelestemur, Y.; Guzelturk, B.; Yerli, O.; Kurum, U.; Yaglioglu, H. G.; Elmali, A.; Demir, Hilmi Volkan
Tunable, high-performance, two-photon absorption (TPA)-based amplified spontaneous emission (ASE) from near-unity quantum efficiency colloidal quantum dots (CQDs) is reported. Besides the absolute spectral tuning of ASE, the relative spectral tuning of ASE peak with respect to spontaneous emission was shown through engineering excitonic interactions in quasi-type-II CdSe/CdS core/shell CQDs. With core shell size adjustments, it was revealed that Coulombic exciton-exciton interactions can be tuned to be attractive (type-I-like) or repulsive (type-II-like) leading to red- or blue-shifted ASE peak, respectively, and that nonshifting ASE can be achieved with the right core shell combinations. The possibility of obtaining ASE at a specific wavelength from both type-I-like and type-II-like CQDs was also demonstrated. The experimental observations were supported by parametric quantum-mechanical modeling, shedding light on the type-tunability. These excitonically engineered CQD-solids exhibited TPA-based ASE threshold as low as 6.5 mJ/cm(2) under 800 nm excitation, displaying one of the highest values of TPA cross-section of 44 660 GM.
Open Access
Colloidal photonics of semiconductor nanocrystals: from polarized color conversion to efficient solar concentration
(2018-07) Güngör, Kıvanç
Effective photon management is pivotal to the success of future photonic applications. The demand for high-performance electronic displays and solar light harvesters has been increasingly growing, ever with high expectations in advancing their power efficiencies. Semiconductor nanocrystals are highly promising for use in such advanced photonic applications. However, conventional device architectures and fabrication methods cannot fully exploit their potential. To address the need for their effective utilization, in this thesis, we proposed and demonstrated novel photon managing methods for colloidal nanocrystals to target polarized color conversion and efficient solar concentration. Nanocrystals possess an unmatched color purity for next-generation displays but color enrichment in displays suffers from the inherent random polarization in their photoluminescence. Instead of clipping the undesired polarization, we show a new class of v-shaped backlight unit (v-BLU) creating Fano resonances to enforce isotropic quantum emitters of the integrated color-conversion nanocrystals to emit polarized light. While enabling a front-panel configuration, the proposed v-BLU of nanocrystals allows for a strong modification of the density of optical states via resonance coupling. This control over the density of states for isotropic quantum dots empowers the realization of high polarization contrast ratios while sustaining their optical transmission. Similar to color conversion, colloidal nanocrystals are also instrumental to light harvesting, in particular using atomically at nanocrystals with their step-like absorption profile making them potentially ideal candidates for luminescent solar concentrators (LSCs). Nevertheless, practically zero Stokes shift in their photoluminescence fundamentally limits their utilization. Here we overcame this limitation by proposing the doping of such colloidal quantum wells inducing a large Stokes shift with near-unity photoluminescence quantum efficiency. We developed and demonstrated high-performance LSC panels of the copper-doped quantum wells outperforming the LSCs of their undoped counterparts and doped quantum dots. The LSCs of such Cu-doped quantum wells offer record optical flux gain compared to other colloids. We believe that the findings presented in this thesis will advance the applications of colloidal nanocrystals boosting the performance of their next-generation photonic devices to unprecedented levels.
Open Access
Generalized theory of förster-type nonradiative energy transfer in nanostructures with mixed dimensionality
(American Chemical Society, 2013-04-16) Hernandez-Martinez, P. L.; Govorov, A. O.; Demir, Hilmi Volkan
Forster-type nonradiative energy transfer (NRET) is widely used, especially utilizing nanostructures in different combinations and configurations. However, the existing well-accepted Forster theory is only for the case of a single particle serving as a donor together with another particle serving as an acceptor. There are also other special cases previously studied; however, there is no complete picture and unified understanding. Therefore, there is a strong need for a complete theory that models Forster-type NRET for the cases of mixed dimensionality including all combinations and configurations. We report a generalized theory for the Forster-type, NRET, which includes the derivation of the effective dielectric function due to the donor in different confinement geometries and the derivation of transfer rates distance dependencies due to the acceptor in different confinement geometries, resulting in a complete picture and understanding of the mixed dimensionality.
Open Access
Nanocrystal skins with exciton funneling for photosensing
(Wiley-VCH Verlag, 2014-03-05) Akhavan, S.; Cihan, A. F.; Bozok, B.; Demir, Hilmi Volkan
Highly photosensitive nanocrystal (NC) skins based on exciton funneling are proposed and demonstrated using a graded bandgap profile across which no external bias is applied in operation for light-sensing. Four types of gradient NC skin devices (GNS) made of NC monolayers of distinct sizes with photovoltage readout are fabricated and comparatively studied. In all structures, polyelectrolyte polymers separating CdTe NC monolayers set the interparticle distances between the monolayers of ligand-free NCs to <1 nm. In this photosensitive GNS platform, excitons funnel along the gradually decreasing bandgap gradient of cascaded NC monolayers, and are finally captured by the NC monolayer with the smallest bandgap interfacing the metal electrode. Time-resolved measurements of the cascaded NC skins are conducted at the donor and acceptor wavelengths, and the exciton transfer process is confirmed in these active structures. These findings are expected to enable large-area GNS-based photosensing with highly efficient full-spectrum conversion.
Open Access
Onion-Like (CdSe)ZnS/CdSe/ZnS quantum-dot-quantum-well heteronanocrystals for investigation of multi-color emission
(Optical Society of America, 2008) Nizamoglu, S.; Demir, Hilmi Volkan
We investigate multi-color spontaneous emission from quantum-dot-quantum-well heteronanocrystals made of onion-like (CdSe) ZnS/CdSe/ZnS ( core) shell/shell/shell structures, with our theoretical results explaining experimental measurements for the first time. In such multi-layered heteronanocrystals, we discover that the carrier localization is tuned from type-1-like to type-2-like localization by controlling CdSe and ZnS shell thicknesses, and that 3-monolayer ZnS barriers are not necessarily sufficient for carrier localization, unlike in conventional ( CdSe) ZnS ( core) shell structures. We demonstrate that exciton localization in distinct layers of ( CdSe) ZnS/CdSe/ZnS heteronanocrystals with high transition probability ( for n=1 states in CdSe core and n=2 states in CdSe shell) is key to their multi-color emission. (c) 2008 Optical Society of America.
Open Access
Plasmonic light-sensitive skins of nanocrystal monolayers
(IOP Publishing, 2013) Akhavan, S.; Gungor, K.; Mutlugun, E.; Demir, Hilmi Volkan
We report plasmonically coupled light-sensitive skins of nanocrystal monolayers that exhibit sensitivity enhancement and spectral range extension with plasmonic nanostructures embedded in their photosensitive nanocrystal platforms. The deposited plasmonic silver nanoparticles of the device increase the optical absorption of a CdTe nanocrystal monolayer incorporated in the device. Controlled separation of these metallic nanoparticles in the vicinity of semiconductor nanocrystals enables optimization of the photovoltage buildup in the proposed nanostructure platform. The enhancement factor was found to depend on the excitation wavelength. We observed broadband sensitivity improvement (across 400-650 nm), with a 2.6-fold enhancement factor around the localized plasmon resonance peak. The simulation results were found to agree well with the experimental data. Such plasmonically enhanced nanocrystal skins hold great promise for large-area UV/visible sensing applications.
Open Access
Resonant nonradiative energy transfer in CdSe/ZnS core/shell nanocrystal solids enhances hybrid white light emitting diodes
(Optical Society of America, 2008) Nizamoglu, S.; Demir, Hilmi Volkan
We propose and demonstrate hybrid white light emitting diodes enhanced with resonant nonradiative energy transfer in CdSe/ZnS core/shell nanocrystal solids integrated on near-UV InGaN/GaN LEDs. We observe a relative quantum efficiency enhancement of 13.2 percent for the acceptor nanocrystals in the energy gradient mixed assembly, compared to the monodisperse phase. This enhancement is attributed to the ability to recycle trapped excitons into nanocrystals using nonradiative energy transfer. We present the time-resolved photoluminescence of these nanocrystal solids to reveal the kinetics of their energy transfer and their steady-state photoluminescence to exhibit the resulting quantum efficiency enhancement.
Open Access
Self-consistent computation of electronic and optical properties of a single exciton in a spherical quantum dot via matrix diagonalization method
(American Institute of Physics, 2009-08-21) Sahin, M.; Nizamoglu, S.; Kavruk, A. E.; Demir, Hilmi Volkan
In this study, we develop and demonstrate an efficient self-consistent calculation schema that computes the electronic structure and optical properties of a single exciton in a spherical quantum dot (QD) with an interacting pair of electron and hole wave functions. To observe modifications on bands, wave functions, and energies due to the attractive Coulomb potential, the full numeric matrix diagonalization technique is employed to determine sublevel energy eigenvalues and their wave functions in effective mass approximation. This treatment allows to observe that the conduction and valance band edges bend, that the electron and hole wave functions strongly localize in the QD, and that the excitonic energy level exhibits redshift. In our approach for the Coulomb term between electron and hole, the Poisson-Schrodinger equations are solved self-consistently in the Hartree approximation. Subsequently, exciton binding energies and associated optical properties are computed. The results are presented as a function of QD radii and photon energies. We conclude that all of these numerical results are in agreement with the experimental studies.
Open Access
Synthesis and characterization of colloidal quantum wells: from simple size-tuned core to complex multi-crown structures
(2018-08) Dede, Didem
As a new class of semiconductor nanocrystals, colloidal quantum wells (CQWs), also commonly known as nanoplatelets (NPLs), exhibit remarkable electronic and optical properties that will potentially nd a wide range of use from nanophotonics to optoelectronics. NPLs feature step-like absorption pro les and discrete emission spectra with giant oscillator strength resulting in high recombination rates. All these features make these atomically- at structures highly attractive for light-harvesting and -generating applications. In this thesis, to understand the size-tuned properties of their two-dimensional architecture, we conducted a systematic study on the core-only NPLs by using a set of 4 monolayer (ML) CdSe cores as our working model and carefully altered their aspect ratio while keeping their lateral area constant. In such a core-only NPL structure, electron and hole are both con ned in the core resulting in type-I electronic band alignment. By decreasing the width of these NPLs to a value comparable to or less than their exciton Bohr radius, we observe additional con nement e ects emerge. Subsequently, by growing CdSe1􀀀xTex alloyed crown around these starting 4 ML CdSe cores, we nd type-II electronic band alignment is obtained. Thanks to their spatially indirect excitons, these core crown NPLs show extraordinarily long radiative lifetimes. Moreover, with the increased absorption cross-section owing to their added crown, high-performance optical gain is achieved via their core/crown heterostructure. However, in this form, their usage is limited since they are unstable in solution forming gels and they exhibit strong tendency to form stacks in lms. To address this problem, here we proposed and developed a multi-crown architecture by additionally growing a CdS crown around the periphery of the type- II heterostructure, enabling excellent optical gain media with enhanced stability. The structural and optical characterizations of the synthesized multi-crown NPLs indicate that this complex architecture holds great promise for making devices in colloidal nanophotonics and optoelectronics.
Open Access
Ultralow threshold one-photon-and two-photon-pumped optical gain media of blue-emitting colloidal quantum dot films
(American Chemical Society, 2014) Guzelturk, B.; Kelestemur, Y.; Akgul, M. Z.; Sharma, V. K.; Demir, Hilmi Volkan
Colloidal quantum dots (QDs) offer advantageous properties as an optical gain media for lasers. Optical gain in the QDs has been shown in the whole visible spectrum, yet it has been intrinsically challenging to realize efficient amplified spontaneous emission (ASE) and lasing in the blue region of the visible spectrum. Here, we synthesize large-sized core/gradient shell CdZnS/ZnS QDs as an efficient optical gain media in the blue spectral range. In this Letter, we demonstrate for the first time that two-photon-absorption-pumped ASE from the blue-emitting QD is achievable with a threshold as low as 6 mJ/cm(2). Utilizing these QDs, we also report one-photon-absorption-pumped ASE at an ultralow threshold of similar to 60 mu J/cm(2), which is comparable to the state-of-the-art red-emitting QD-based gain media. This one-photon-pumped ASE threshold is an order of magnitude better than that of the previously reported best blue-emitting QD-based gain media.