Browsing by Subject "Nonradiative energy transfer"

Now showing 1 - 20 of 23

Open Access
Broadband optical transparency in plasmonic nanocomposite polymer films via exciton-plasmon energy transfer
(OSA - The Optical Society, 2016) Dhama R.; Rashed, A. R.; Caligiuri V.; El Kabbash M.; Strangi, G.; De Luca A.
Inherent absorptive losses affect the performance of all plasmonic devices, limiting their fascinating applications in the visible range. Here, we report on the enhanced optical transparency obtained as a result of the broadband mitigation of optical losses in nanocomposite polymeric films, embedding core-shell quantum dots (CdSe@ZnS QDs) and gold nanoparticles (Au-NPs). Exciton-plasmon coupling enables non-radiative energy transfer processes from QDs to metal NPs, resulting in gain induced transparency of the hybrid flexible systems. Experimental evidences, such as fluorescence quenching and modifications of fluorescence lifetimes confirm the presence of this strong coupling between plexcitonic elements. Measures performed by means of an ultra-fast broadband pump-probe setup demonstrate loss compensation of gold NPs dispersed in plastic network in presence of gain. Furthermore, we compare two films containing different concentrations of gold NPs and same amount of QDs, to investigate the role of acceptor concentration (Au-NPs) in order to promote an effective and efficient energy transfer mechanism. Gain induced transparency in bulk systems represents a promising path towards the realization of loss compensated plasmonic devices. © 2016 Optical Society of America.
Open Access
Colloidal optoelectronics of self-assembled quantum well superstructures
(2020-06) Erdem, Onur
Advances 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.
Open Access
Colloidal quantum dot light-emitting diodes employing phosphorescent small organic molecules as efficient exciton harvesters
(American Chemical Society, 2014) Mutlugun, E.; Guzelturk, B.; Abiyasa, A. P.; Gao, Y.; Sun X. W.; Demir, Hilmi Volkan
Nonradiative energy transfer (NRET) is an alternative excitation mechanism in colloidal quantum dot (QD) based electroluminescent devices (QLEDs). Here, we develop hybrid highly spectrally pure QLEDs that facilitate energy transfer pumping via NRET from a phosphorescent small organic molecule-codoped charge transport layer to the adjacent QDs. A partially codoped exciton funnelling electron transport layer is proposed and optimized for enhanced QLED performance while exhibiting very high color purity of 99%. These energy transfer pumped hybrid QLEDs demonstrate a 6-fold enhancement factor in the external quantum efficiency over the conventional QLED structure, in which energy transfer pumping is intrinsically weak.
Open Access
Excitonic enhancement of nonradiative energy transfer to bulk silicon with the hybridization of cascaded quantum dots
(AIP, 2013) Yeltik A.; Guzelturk, B.; Hernandez-Martinez, P. L.; Akhavan S.; Demir, Hilmi Volkan
We report enhanced sensitization of silicon through nonradiative energy transfer (NRET) of the excitons in an energy-gradient structure composed of a cascaded bilayer of green- and red-emitting CdTe quantum dots (QDs) on bulk silicon. Here NRET dynamics were systematically investigated comparatively for the cascaded energy-gradient and mono-dispersed QD structures at room temperature. We show experimentally that NRET from the QD layer into silicon is enhanced by 40% in the case of an energy-gradient cascaded structure as compared to the mono-dispersed structures, which is in agreement with the theoretical analysis based on the excited state population-depopulation dynamics of the QDs. © 2013 AIP Publishing LLC.
Open Access
Excitonic improvement of colloidal nanocrystals in salt powder matrix for quality lighting and color enrichment
(OSA - The Optical Society, 2016) Erdem, T.; Soran-Erdem, Z.; Kelestemur, Y.; Gaponik, N.; Demir, Hilmi Volkan
Here we report excitonic improvement in color-converting colloidal nanocrystal powders enabled by co-integrating nonpolar greenand red-emitting nanocrystal energy transfer pairs into a single LiCl salt matrix. This leads to nonradiative energy transfer (NRET) between the cointegrated nanocrystals in the host matrix. Here we systematically studied the resulting NRET process by varying donor and acceptor concentrations in the powders. We observed that NRET is a strong function of both of the nanocrystal concentrations and that NRET efficiency increases with increasing acceptor concentration. Nevertheless, with increasing donor concentration in the powders, NRET efficiency was found to first increase (up to a maximum level of 53.9%) but then to decrease. As a device demonstrator, we employed these NRET-improved nanocrystal powders as color-converters on blue light-emitting diodes (LEDs), with the resulting hybrid LED exhibiting a luminous efficiency >70 lm/Welect . The proposed excitonic nanocrystal powders potentially hold great promise for quality lighting and color enrichment applications.
Open Access
Förster-type nonradiative energy transfer directed from colloidal quantum dots to epitaxial quantum wells for light harvesting applications
(Optical Society of America, 2011) Nizamoğlu, Sedat; Sarı, Emre; Baek J.-H.; Lee I.-H.; Demir, Hilmi Volkan
We report on Frster-type nonradiative energy transfer directed from CdSe/ZnS core/shell quantum dots to InGaN/GaN quantum wells with 69.6% efficiency at 1.527 ns-1 rate at room temperature for potential light harvesting and solar cells applications. © 2011 OSA.
Open Access
Förster-type resonance energy transfer (FRET): Applications
(Springer Verlag, 2017) Demir, Hilmi Volkan; Hernández Martínez, Pedro Ludwig; Govorov, Alexander
In this chapter, we present several applications of Förster-type nonradiative energy transfer (FRET) related phenomena. In particular, we review light generation and light harvesting applications as well as bio-applications. © 2017, The Author(s).
Open Access
Green/yellow solid state lighting via radiative and nonradiative energy transfer involving colloidal semiconductor nanocrystals
(IEEE, 2009-08-05) Nizamoglu, S.; Sari, E.; Baek, J. H.; Lee, I. H; Demir, Hilmi Volkan
LEDs made of In(x)Ga(1-x)N and (Al(x)Ga(1-x))(1-y)In(y)P suffer from significantly reduced quantum efficiency and luminous efficiency in the green/yellow spectral ranges. To address these problems, we present the design, growth, fabrication, hybridization, and characterization of proof-of-concept green/yellow hybrid LEDs that utilize radiative and nonradiative [Forster resonance energy transfer (FRET)] energy transfers in their colloidal semiconductor nanocrystals (NCs) integrated on near-UV LEDs. In our first NC-LED, we realize a color-converted LED that incorporate green-emitting CdSe/ZnS core/shell NCs (lambda(PL) = 548 nm) on near-UV InGaN/GaN LEDs (lambda(EL) = 379 nm). In our second NC-LED, we implement a color-converted FRET-enhanced LED. For that, we hybridize a custom-design assembly of cyan-and green-emitting CdSe/ZnS core/shell NCs (lambda(PL) = 490 and 548 nm) on near-UV LEDs. Using a proper mixture of differently sized NCs, we obtain a quantum efficiency enhancement of 9% by recycling trapped excitons via FRET. With FRET-NC-LEDs, we show that it is possible to obtain a luminous efficacy of 425 lm/W(opt) and a luminous efficiency of 94 lm/W, using near-UV LEDs with a 40% external quantum efficiency. Finally, we investigate FRET-converted light-emitting structures that use nonradiative energy transfer directly from epitaxial quantum wells to colloidal NCs. These proof-of-concept demonstrations show that FRET-based NC-LEDs hold promise for efficient solid-state lighting in green/yellow.
Open Access
Highly efficient nonradiative energy transfer using charged CdSe/ZnS nanocrystals for light-harvesting in solution
(American Institute of Physics, 2009-07-20) Mutlugün, E.; Nizamoğlu, S.; Demir, Hilmi Volkan
We propose and demonstrate highly efficient nonradiative Förster resonance energy transfer (FRET) facilitated by the use of positively charged CdSe/ZnS core-shell nanocrystals (NCs) for light-harvesting in solution. With rhodamine B dye molecules used as the acceptors, our time-resolved photoluminescence measurements show substantial lifetime modifications of these amine-functionalized NC donors from 18.16 to 1.88 ns with FRET efficiencies >90% in solution. These strong modifications allow for light-harvesting beyond the absorption spectral range of the acceptor dye molecules.
Open Access
Innovative hybrid composite nanomaterials
(2016-09) Erdem, Zeliha Soran
Digital lighting and bio-imaging are two emerging crucial research fields. Nanotechnology stands in the center of these applications by providing nano-scale particles possessing large surface-to-volume ratios, high effciency, and low toxicity while allowing for functionalization, effcient quality lighting and improved biocompatible bio-imaging. Some of the frequently employed nanoparticles in optoelectronics and imaging are colloidal semiconductor quantum dots, colloidal conjugated polymer nanoparticles, and colloidal iron oxide nanoparticles, all of which we have studied using colloidal approaches to make hybrid composites for lighting and imaging in this thesis. Fluorescent inorganic nanoparticles of colloidal quantum dots (QDs) attract significant interest for many optoelectronic and biomedical applications. Although they possess numerous advantages including broad absorption band, high quantum yield, and narrow emission spectrum, there are serious concerns on their recycling due to their cadmium-based composition. Alternatively, relatively low toxic organic uorescent polymer nanoparticles or oligomer nanoparticles have stepped forward. However, their reduced emission effciency and stability in solid state is an important limitation for their use in wide-spread solid-state lighting applications. To address these problems, in the first part of this thesis, we proposed and demonstrated the design of new hybrid composite material systems of oligomer nanoparticles to be used in solid-state lighting. We first showed that the emission effciency and stability of the oligomer nanoparticles in solid state are significantly improved based on our proposed crystallization technique. Here, using this simple and low-cost approach, oligomer nanoparticle monoliths were obtained from the powders of these crystals. Despite the disadvantages of using QDs, their high quantum effciency and narrow-band emission still make them a valuable asset for solid-state lighting. However, the decrease in solid-film effciencies is still an important issue to be addressed. With this perspective, in this thesis we utilized the incorporation of QDs into crystalline matrices allowing for the nonradiative energy transfer (NRET) to improve the emission capability of the nano-emitters. Since it is an interesting crystalline semiconductor organic molecule, we employed anthracene as the host donor medium and incorporated the quantum dots being exciton acceptors. Here, we systematically investigated the NRET from each anthracene emission peak to QDs and demonstrated the use of this composite system on LEDs as color converters and the polarization ratio change of quantum dots within this crystal system. Magnetic resonance imaging (MRI), for which we also developed colloidal contrast agents using nanoparticles (NPs) as the second part of this thesis, is a powerful diagnostic tool providing good soft tissue contrast and high spatial resolution. It produces T1- and T2-weighted images, in which the region of interest is observed as brighter and darker contrast, respectively. Superparamagnetic iron oxide (IO) NPs are an important member of T2-weighted contrast agents possessing low toxicity. However, they suer from poor anatomic details due to their darker contrast. Therefore, combining T1- and T2-weighted features in a single IO NP (dual-modal contrast) is a major step for improving MRI contrast. In order to meet the requirement for dual-modal contrast agents, which possess both T1- and T2-weighted imaging capability, in this thesis we synthesized highly monodisperse superparamagnetic cubic IO NPs. Magnetic characterizations along with in vivo MRI experiments demonstrated that these nanoparticles hold great promise for dual-modal imaging. This increased dual-modal eect without paramagnetic material doping or decreasing the size of nanoparticles smaller than 5 nm directed us to understand the relation of the T1 and T2 relaxations depending on the IO NP size and shape. Here, we showed the presence of intrinsic paramagnetic phase in magnetite IO NPs. Moreover, we demonstrated that this contribution is higher in IO NPs possessing cubic shape compared to the spherical counterparts, which explains the increased dual-modal effect in the monodisperse superparamagnetic nanocubes.
Open Access
Liquid interface self-assembly of colloidal nanoplatelets for optoelectronics
(Springer Singapore, 2022-10-28) Erdem, Onur; Demir, Hilmi Volkan
In this chapter, we discuss how liquid interface self-assembly can contribute to the utilization of colloidal semiconductor nanoplatelets in optoelectronics. Self-assembled nanoplatelet mono- or multilayers can be used as two-dimensional optically active waveguides, gain media of ultra-thin lasers, or energy transfer-based photosensitizers.
Open Access
Nanocrystal integrated light emitting diodes based on radiative and nonradiative energy transfer for the green gap
(IEEE, 2009) Nizamoğlu, Sedat; Sarı, Emre; Baek J.-H.; Lee I.-H.; Demir, Hilmi Volkan
Recently the photometric conditions for ultra-efficient solid-state lighting have been discussed [1-2]. These studies show that a luminous efficacy of optical radiation at 408 lm/Wopt and a color rendering index (CRI) of 90 at a correlated color temperature (CCT) of 3000 K are achievable at the same time. For this purpose light emitting diodes (LEDs) emitting in blue, green, yellow, and red colors at 463, 530, 573, and 614 nm with relative optical power levels of 1/8, 2/8, 2/8, and 3/8, are required, respectively [1-2]. Although InxGa1-xN material system is capable to cover the whole visible by changing the In composition (x), it is technically extremely challenging to obtain efficient green/yellow light emitting diodes especially at those wavelengths (i.e., at 530 nm and 573 nm, respectively) due to reduced internal quantum efficiency [2-4]. Furthermore, by using the (Al xGa1-x)1-yInyP quaternary alloy it is also possible to cover from 650 nm to 580 nm. However, the efficiencies significantly decrease towards green. Therefore, there exists a significant gap in the green-yellow spectral regions (known as "the green gap") to make efficient light emitting diodes. To address this green gap problem, we propose and demonstrate proof-of-concept nanocrystal (NCs) hybridized green/yellow light emitting diodes that rely on both radiative energy transfer and nonradiative energy transfer (i.e., FRET-Förster resonance energy transfer) for color conversion on near-ultraviolet (near-UV) LEDs.
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
Nonradiative energy transfer in colloidal CdSe nanoplatelet films
(Royal Society of Chemistry, 2015) Güzeltürk, B.; Olutas M.; Delikanlı, S.; Keleştemur, Y.; Erdem, O.; Demir, Hilmi Volkan
Nonradiative energy transfer (NRET) has been extensively studied in colloidal nanocrystal (quantum dots) and nanorod (quantum wires) assemblies. In this work, we present the first account of spectroscopic evidence of NRET in solid thin films of CdSe based colloidal nanoplatelets (NPLs), also known as colloidal quantum wells. The NRET was investigated as a function of the concentration of two NPL populations with different vertical thicknesses via steady state and time resolved spectroscopy. NRET takes place from the NPLs with smaller vertical thickness (i.e., larger band gap) to the ones with a larger vertical thickness (i.e., smaller band gap) with efficiency up to ∼60%. Here, we reveal that the NRET efficiency is limited in these NPL solid film assemblies due to the self-stacking of NPLs within their own population causing an increased distance between the donor-acceptor pairs, which is significantly different to previously studied colloidal quantum dot based architectures for nonradiative energy transfer. © The Royal Society of Chemistry 2015.
Open Access
Observation of biexcitons in the presence of trions generated via sequential absorption of multiple photons in colloidal quantum dot solids
(IEEE, 2012) Cihan, Ahmet Fatih; Hernandez-Martinez Pedro L.; Kelestemur, Yusuf; Demir, Hilmi Volkan
Multi exciton generation (MEG) and multi exciton recombination (MER) in semiconductor quantum dots (QDs) have recently attracted significant scientific interest as a possible means to improve device efficiencies [1-5]. Convenient bandgap tunability, easy colloidal synthesis, and solution-based processability of these QDs make them further attractive for such device applications using MEG and MER. For example, recent theoretical and experimental studies have shown that MEG enables >100% peak external quantum efficiency where the generated multi excitons (MEs) are collected in a simple QD solar cell structure [1]. Furthermore, MEG has also been shown in QD photodetectors exhibiting substantially increased photocurrent levels [2]. Another promising application for MEs is the use of QDs as an alternative gain medium based on MER for lasers. Although MEG is very promising and supported with quite persuasive reports, there are still some debatable issues that need to be clarified. One of the issues that have generated great debates in the field has been the confusion of MER with the recombination of trions, which takes place in photocharged QDs. To utilize MEG and MER in practical devices such as QD solar cells and QD lasing devices, these phenomena need to be well understood. Here, we showed distinct spectrally-resolved temporal behavior of biexciton (BX), single exciton (X) and trion radiative recombinations in near unity quantum yield (QY) quasi-type II CdSe/CdS core/shell nanocrystal QDs. Upon sequential absorption of multiple photons, the extraction of Xs, BXs, and trions were achieved using time correlated single photon counting (TCSPC) measurements performed on low concentration thin film samples of these QDs at different emission wavelengths. The QDs were embedded in PMMA medium to obtain homogeneous samples and avoid Förster-type nonradiative energy transfer (NRET) between them. Here to extract Xs, BXs, and trions, we devised a new analysis approach for the time decays of the QDs that allowed us to attribute the physical events to their corresponding time decay terms, which were further verified with their excitation intensity dependencies [6]. © 2012 IEEE.
Open Access
Peptide-mediated constructs of quantum dot nanocomposites for enzymatic control of nonradiative energy transfer
(American Chemical Society, 2011) Seker U.O.S.; Ozel, T.; Demir, Hilmi Volkan
A bottom-up approach for constructing colloidal semiconductor quantum dot (QDot) nanocomposites that facilitate nonradiative Förster-type resonance energy transfer (FRET) using polyelectrolyte peptides was proposed and realized. The electrostatic interaction of these polypeptides with altering chain lengths was probed for thermodynamic, structural, and morphological aspects. The resulting nanocomposite film was successfully cut with the protease by digesting the biomimetic peptide layer upon which the QDot assembly was constructed. The ability to control photoluminescence decay lifetime was demonstrated by proteolytic enzyme activity, opening up new possibilities for biosensor applications.
Open Access
Phonon-assisted nonradiative energy transfer from colloidal quantum dots to monocrystalline bulk silicon
(IEEE, 2012) Yeltik, Aydan; Güzeltürk, Burak; Hernandez-Martinez, Pedro L.; Demir, Volkan Demir
Silicon is one of the most dominant materials in photovoltaics. To increase optical absorption of silicon solar cells, colloidal quantum dots (QDs) have been proposed as a good sensitizer candidate owing to their favorably high absorption cross-section and tunable emission and absorption properties. To this end, QD sensitization of silicon has previously been studied by mostly facilitating radiative energy transfer (RET) [1,2]. Although RET based sensitization has achieved a considerable increase in conversion efficiencies in silicon photovoltaics, RET is fundamentally limited due to the effective coupling problem of emitted photons to silicon. Alternatively, nonradiative energy transfer (NRET), which relies on near field dipole-dipole coupling [3], has been shown to be feasible in sensitizer-silicon hybrid systems [4-8]. Although colloidal QDs as a sensitizer have been used to facilitate NRET into silicon, the detailed mechanisms of NRET to an indirect bandgap nonluminecent material, together with the role of phonon assistance and temperature activation, have not been fully understood to date. In this study, we propose a QD-silicon nanostructure hybrid platform to study the NRET dynamics as a function of temperature for distinct separation thicknesses between the donor QDs and the acceptor silicon plane. Here, we show NRET from colloidal QDs to bulk Si using phonon assisted absorption, developing its physical model to explain temperature-dependent lifetime dynamics of NRET in these QD-Si hybrids. © 2012 IEEE.
Open Access
Physics of nonradiative energy transfer in the complex media of 0D, 2D and 3D materials
(2016-07) Yeltik, Aydan
Quantum-confined colloidal nanostructures with strong excitonic properties have emerged as promising light harvesting components in photonics and optoelectronics over the past 20 years. With their favorable photophysical characteristics, three-dimensional-confined colloidal quantum dots and 2D-confined colloidal quantum wells have garnered great attention in the fields ranging from biology and chemistry to physics and engineering. It is technologically significant to utilize the key characteristics of these brightly luminescent nanomaterials through hybridizing and/or interfacing with various technological materials including 3D bulk silicon, graphene based 2D structures such as graphene oxide and reduced graphene oxide, and 2D layered transition metal dichalcogenides such as molybdenum disulphide. Compelling partnership of these appealing materials can be achieved through the nonradiative energy transfer (NRET), which is a phenomenon involving both the exciton and charge transfer mechanisms. Along with the hybrids of low dimensional particles with the conventional bulk materials, the closely interacting structures of these colloidal and layered nanomaterials have widespread interest at both the fundamental science and application levels. From these physical and technological points of view, in this thesis, we addressed important scientific problems and proposed innovative solutions including both the experimental and theoretical approaches in interfacing complex media of 0D, 2D and 3D materials and showing strong NRET interactions. Our key achievements include high excitonic enhancement in silicon and graphene based materials with the integration of nanoparticles, comprehensive photophysical investigation of the newly emerging nanomaterials and successful tailoring of the colloidal nanostructures to the next-generation optoelectronic applications.
Open Access
Plasmon-enhanced energy transfer in photosensitive nanocrystal device
(American Chemical Society, 2017) Akhavan S.; Akgul, M. Z.; Hernandez-Martinez, P. L.; Demir, Hilmi Volkan
Förster resonance energy transfer (FRET) interacted with localized surface plasmon (LSP) gives us the ability to overcome inadequate transfer of energy between donor and acceptor nanocrystals (NCs). In this paper, we show LSP-enhanced FRET in colloidal photosensors of NCs in operation, resulting in substantially enhanced photosensitivity. The proposed photosensitive device is a layered self-assembled colloidal platform consisting of separated monolayers of the donor and the acceptor colloidal NCs with an intermediate metal nanoparticle (MNP) layer made of gold interspaced by polyelectrolyte layers. Using LBL assembly, we fabricated and comparatively studied seven types of such NC-monolayer devices (containing only donor, only acceptor, Au MNP-donor, Au MNP-acceptor, donor-acceptor bilayer, donor-Au MNP-acceptor trilayer, and acceptor-Au MNP-donor reverse trilayer). In these structures, we revealed the effect of LSP-enhanced FRET and exciton interactions from the donor NCs layer to the acceptor NCs layer. Compared to a single acceptor NC device, we observed a significant extension in operating wavelength range and a substantial photosensitivity enhancement (2.91-fold) around the LSP resonance peak of Au MNPs in the LSP-enhanced FRET trilayer structure. Moreover, we present a theoretical model for the intercoupled donor-Au MNP-acceptor structure subject to the plasmon-mediated nonradiative energy transfer. The obtained numerical results are in excellent agreement with the systematic experimental studies done in our work. The potential to modify the energy transfer through mastering the exciton-plasmon interactions and its implication in devices make them attractive for applications in nanophotonic devices and sensors.
Open Access
Singlet and Triplet Exciton Harvesting in the Thin Films of Colloidal Quantum Dots Interfacing Phosphorescent Small Organic Molecules
(American Chemical Society, 2014) Guzelturk, B.; Hernandez Martinez P.L.; Zhao, D.; Sun X.W.; Demir, Hilmi Volkan
Efficient nonradiative energy transfer is reported in an inorganic/organic thin film that consists of a CdSe/ZnS core/shell colloidal quantum dot (QD) layer interfaced with a phosphorescent small organic molecule (FIrpic) codoped fluorescent host (TCTA) layer. The nonradiative energy transfer in these thin films is revealed to have a cascaded energy transfer nature: first from the fluorescent host TCTA to phosphorescent FIrpic and then to QDs. The nonradiative energy transfer in these films enables very efficient singlet and triplet state harvesting by the QDs with a concomitant fluorescence enhancement factor up to 2.5-fold, while overall nonradiative energy transfer efficiency is as high as 95%. The experimental results are successfully supported by the theoretical energy transfer model developed here, which considers exciton diffusion assisted Förster-type near-field dipole-dipole coupling within the hybrid films. © 2014 American Chemical Society.