Organic-Inorganic Composites of Semiconductor Nanocrystals for Efficient Excitons

Cataloged from PDF version of article.Nanocomposites of colloidal semiconductor nanocrystals integrated into conjugated polymers are the key to soft-material hybrid optoelectronics, combining advantages of both plastics and particles. Synergic combination of the favorable properties in the hybrids of colloidal nanocrystals and conjugated polymers offers enhanced performance and new functionalities in light-generation and light-harvesting applications, where controlling and mastering the excitonic interactions at the nanoscale are essential. In this Perspective, we highlight and critically consider the excitonic interactions in the organic inorganic nanocomposites to achieve highly efficient exciton transfer through rational design of the nanocomposites. The use of strong excitonic interactions in optoelectronic devices can trigger efficiency breakthroughs in hybrid optoelectronics

Near-Field Energy Transfer Using Nanoemitters For Optoelectronics

Effective utilization of excitation energy in nanoemitters requires control of exciton flow at the nanoscale. This can be readily achieved by exploiting near-field nonradiative energy transfer mechanisms such as dipole-dipole coupling (i.e., Förster resonance energy transfer) and simultaneous two-way electron transfer via exchange interaction (i.e., Dexter energy transfer). In this feature article, we review nonradiative energy transfer processes between emerging nanoemitters and exciton scavengers. To this end, we highlight the potential of colloidal semiconductor nanocrystals, organic semiconductors, and two-dimensional materials as efficient exciton scavengers for light harvesting and generation in optoelectronic applications. We present and discuss unprecedented exciton transfer in nanoemitter–nanostructured semiconductor composites enabled by strong light–matter interactions. We elucidate remarkably strong nonradiative energy transfer in self-assembling atomically flat colloidal nanoplatelets. In addition, we underscore the promise of organic semiconductor–nanocrystal hybrids for spin-triplet exciton harvesting via Dexter energy transfer. These efficient exciton transferring hybrids will empower desired optoelectronic properties such as long-range exciton diffusion, ultrafast multiexciton harvesting, and efficient photon upconversion, leading to the development of excitonic optoelectronic devices such as exciton-driven light-emitting diodes, lasers, and photodetectors. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinhei

Type-tunable amplified spontaneous emission from core-seeded CdSe/CdS nanorods controlled by exciton-exciton interaction

Cataloged from PDF version of article.Type-tunable optical gain performance of core-seeded CdSe/CdS nanorods is studied via two-photon optical pumping. Controlling the exciton-exciton interaction by varying the core and shell size, blue-shifted and red-shifted modes of amplified spontaneous emission are systematically demonstrated and their type attributions are verified by time-resolved emission kinetics

Large-area semi-transparent light-sensitive nanocrystal skins

Cataloged from PDF version of article.We report a large-area, semi-transparent, light-sensitive nanocrystal skin (LS-NS) platform consisting of single monolayer colloidal nanocrystals. LS-NS devices, which were fabricated over areas up to 48 cm(2) using spray-coating and several cm-squares using dip-coating, are operated on the principle of photogenerated potential buildup, unlike the conventional charge collection. Implementing proof-of-concept devices using CdTe nanocrystals with ligand removal, we observed a substantial sensitivity enhancement factor of similar to 73%, accompanied with a 3-fold faster response time (<100 ms). With fully sealed nanocrystal monolayers, LS-NS is found to be highly stable under ambient conditions, promising for low-cost large-area UV/visible sensing in windows and facades of smart buildings. (C) 2012 Optical Society of Americ

Stacking in Colloidal Nanoplatelets: Tuning Excitonic Properties

Cataloged from PDF version of article.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

Efficient nonradiative energy transfer from InGaN/GaN nanopillars to CdSe/ZnS core/shell nanocrystals

Cataloged from PDF version of article.In this study, we propose and demonstrate efficient electron-hole pair injection from InGaN/GaN multiple quantum well nanopillars (MQW-NPs) to CdSe/ZnS core/shell nanocrystal quantum dots (NQDs) via Forster-type nonradiative energy transfer. For that we hybridize blue-emitting MQW-NPs with red-emitting NQDs and the resultant exciton transfer reaches a maximum rate of (0.192 ns)(-1) and a maximum efficiency of 83.0%. By varying the effective bandgap of core/shell NQDs, we conveniently control and tune the excitonic energy transfer rate for these NQD integrated hybrids, and our measured and computed exciton transfer rates are found to be in good agreement for all hybrid cases. (C) 2011 American Institute of Physics

Light-Induced Currents at Domain Walls in Multiferroic BiFeO3.

Multiferroic BiFeO3 (BFO) films with spontaneously formed periodic stripe domains can generate above-gap open circuit voltages under visible light illumination; nevertheless the underlying mechanism behind this intriguing optoelectronic response has not been understood to date. Here, we make contact-free measurements of light-induced currents in epitaxial BFO films via detecting terahertz radiation emanated by these currents, enabling a direct probe of the intrinsic charge separation mechanisms along with quantitative measurements of the current amplitudes and their directions. In the periodic stripe samples, we find that the net photocurrent is dominated by the charge separation across the domain walls, whereas in the monodomain samples the photovoltaic response arises from a bulk shift current associated with the non-centrosymmetry of the crystal. The peak current amplitude driven by the charge separation at the domain walls is found to be 2 orders of magnitude higher than the bulk shift current response, indicating the prominent role of domain walls acting as nanoscale junctions to efficiently separate photogenerated charges in the stripe domain BFO films. These findings show that domain-wall-engineered BFO thin films offer exciting prospects for ferroelectric-based optoelectronics, as well as bias-free strong terahertz emitters

Phonon-Assisted Exciton Transfer into Silicon Using Nanoemitters: The Role of Phonons and Temperature Effects in Forster Resonance Energy Transfer

Cataloged from PDF version of article.We study phonon-assisted Forster resonance energy transfer (FRET) into an indirect band-gap semiconductor using nanoemitters. The unusual temperature dependence of this energy transfer, which is measured using the donor nanoemitters of quantum dot (QD) layers integrated on the acceptor monocrystalline bulk silicon as a model system, is predicted by a phonon-assisted exciton transfer model proposed here. The model includes the phonon-mediated optical properties of silicon, while considering the contribution from the multimonolayer-equivalent QD film to the nonradiative energy transfer, which is derived with a d(-3) distance dependence. The FRET efficiencies are experimentally observed to decrease at cryogenic temperatures, which are well explained by the model considering the phonon depopulation in the indirect band-gap acceptor together with the changes in the quantum yield of the donor. These understandings will be crucial for designing FRET-enabled sensitization of silicon based high-efficiency excitonic systems using nanoemitters

Lateral Size-Dependent Spontaneous and Stimulated Emission Properties in Colloidal CdSe Nanoplatelets

Cataloged from PDF version of article.Here, 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

Excitonic enhancement of nonradiative energy transfer to bulk silicon with the hybridization of cascaded quantum dots

Cataloged from PDF version of article.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. (C) 2013 AIP Publishing LLC