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Temperature and Composition Dependent Optical Properties of CdSe/CdS Dot/Rod-Based Aerogel Networks.

ABSTRACT: Employing nanocrystals (NCs) as building blocks of porous aerogel network structures allows the conversion of NC materials into macroscopic solid structures while conserving their unique nanoscopic properties. Understanding the interplay of the network formation and its influence on these properties like size-dependent emission is a key to apply techniques for the fabrication of novel nanocrystal aerogels. In this work, CdSe/CdS dot/rod NCs possessing two different CdSe core sizes were synthesized and converted into porous aerogel network structures. Temperature-dependent steady-state and time-resolved photoluminescence measurements were performed to expand the understanding of the optical and electronic properties of these network structures generated from these two different building blocks and correlate their optical with the structural properties. These investigations reveal the influence of network formation and aerogel production on the network-forming nanocrystals. Based on the two investigated NC building blocks and their aerogel networks, mixed network structures with various ratios of the two building blocks were produced and likewise optically characterized. Since the different building blocks show diverse optical response, this technique presents a straightforward way to color-tune the resulting networks simply by choosing the building block ratio in connection with their quantum yield.

SUBMITTER: Rusch P

PROVIDER: S-EPMC9299188 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Optical Alignment and Optical Orientation of Excitons in CdSe/CdS Colloidal Nanoplatelets.

Project description:Optical alignment and optical orientation of excitons are studied experimentally on an ensemble of core/shell CdSe/CdS colloidal nanoplatelets. Linear and circular polarization of photoluminescence during resonant excitation of excitons is measured at cryogenic temperatures and with magnetic fields applied in the Faraday geometry. The developed theory addresses the optical alignment and optical orientation of excitons in colloidal nanocrystals, taking into account both bright and dark exciton states in the presence of strong electron-hole exchange interaction and the random in-plane orientation of nanoplatelets within the ensemble. Our theoretical analysis of the obtained experimental data allows us to evaluate the exciton fine structure parameters, the g-factors, and the spin lifetimes of the bright and dark excitons. The optical alignment effect enables the identification of the exciton and trion contributions to the emission spectrum, even in the absence of their clear separation in the spectra.

| S-EPMC10489814 | biostudies-literature

Reversible Charge-Carrier Trapping Slows Forster Energy Transfer in CdSe/CdS Quantum-Dot Solids.

Project description:The dynamics of photoluminescence (PL) from nanocrystal quantum dots (QDs) is significantly affected by the reversible trapping of photoexcited charge carriers. This process occurs after up to 50% of the absorption events, depending on the type of QD considered, and can extend the time between the photoexcitation and relaxation of the QD by orders of magnitude. Although many optoelectronic applications require QDs assembled into a QD solid, until now, reversible trapping has been studied only in (ensembles of) spatially separated QDs. Here, we study the influence of reversible trapping on the excited-state dynamics of CdSe/CdS core/shell QDs when they are assembled into close-packed "supraparticles". Time- and spectrally resolved photoluminescence (PL) measurements reveal competition among spontaneous emission, reversible charge-carrier trapping, and Förster resonance energy transfer between the QDs. While Förster transfer causes the PL to red-shift over the first 20-50 ns after excitation, reversible trapping stops and even reverses this trend at later times. We can model this behavior with a simple kinetic Monte Carlo simulation by considering that charge-carrier trapping leaves the QDs in a state with zero oscillator strength in which no energy transfer can occur. Our results highlight that reversible trapping significantly affects the energy and charge-carrier dynamics for applications in which QDs are assembled into a QD solid.

| S-EPMC6139578 | biostudies-literature

Covalent Protein Labeling and Improved Single-Molecule Optical Properties of Aqueous CdSe/CdS Quantum Dots.

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| S-EPMC9933437 | biostudies-literature

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Project description:Room-temperature exciton-polariton Bose-Einstein condensation (BEC), a phase transition to single quantum state with strong nonlinearity, provides a new strategy for coherent light sources and ultralow threshold optic switches. In this work, colloidal CdSe/CdS 2D nanoplatelets are embedded into a microcavity, and exciton-polariton BEC is realized with an ultralow threshold of 0.5 µJ cm-2 at room temperature. The superlinear power-dependent emission, macroscopic occupation of the ground state, strong blueshift and broadening of the emission peak, and long-range coherence strongly confirm the realization of the polariton laser. This work suggests considerable prospects for colloidal nanoplatelets in low-cost, high-performance polariton devices, and coherent light sources.

| S-EPMC9218774 | biostudies-literature

Biological Synthesis of CdS/CdSe Core/Shell Nanoparticles and Its Application in Quantum Dot Sensitized Solar Cells.

Project description:In the present work, we report the use of bacterial cells for the production of CdS/CdSe Core/Shell quantum dots (QDs), a complex nanostructure specially designed to improve their performance as photosensitizer in photovoltaic devices. The method requires the incorporation of L-cysteine, CdCl2 and Na2SeO3 to Escherichia coli cultures and allows a tight control of QDs properties. The obtained CdS/CdSe QDs were photophysically and structurally characterized. When compared to CdS QDs, the classical shift in the UV-visible spectra of Core/Shell nanostructures was observed in CdS/CdSe QDs. The nanosize, structure, and composition of Core/Shell QDs were confirmed by TEM and EDS analysis. QDs presented a size of approximately 12 nm (CdS) and 17 nm (CdS/CdSe) as determined by dynamic light scattering (DLS), whereas the fourier transform infrared (FTIR) spectra allowed to distinguish the presence of different biomolecules bound to both types of nanoparticles. An increased photostability was observed in CdS/CdSe nanoparticles when compared to CdS QDs. Finally, biosynthesized CdS/CdSe Core/Shell QDs were used as photosensitizers for quantum dots sensitized solar cells (QDSSCs) and their photovoltaic parameters determined. As expected, the efficiency of solar cells sensitized with biological CdS/CdSe QDs increased almost 2.5 times when compared to cells sensitized with CdS QDs. This work is the first report of biological synthesis of CdS/CdSe Core/Shell QDs using bacterial cells and represents a significant contribution to the development of green and low-cost photovoltaic technologies.

| S-EPMC6637821 | biostudies-literature

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Project description:Colloidal two-dimensional (2D) nanoplatelet heterostructures are particularly interesting as they combine strong confinement of excitons in 2D materials with a wide range of possible semiconductor junctions due to a template-free, solution-based growth. Here, we present the synthesis of a ternary 2D architecture consisting of a core of CdSe, laterally encapsulated by a type-I barrier of CdS, and finally a type-II outer layer of CdTe as so-called crown. The CdS acts as a tunneling barrier between CdSe- and CdTe-localized hole states, and through strain at the CdS/CdTe interface, it can induce a shallow electron barrier for CdTe-localized electrons as well. Consequently, next to an extended fluorescence lifetime, the barrier also yields emission from CdSe and CdTe direct transitions. The core/barrier/crown configuration further enables two-photon fluorescence upconversion and, due to a high nonlinear absorption cross section, even allows to upconvert three near-infrared photons into a single green photon. These results demonstrate the capability of 2D heterostructured nanoplatelets to combine weak and strong confinement regimes to engineer their optoelectronic properties.

| S-EPMC7199781 | biostudies-literature

Performance Enhancement of CdS/CdSe Quantum Dot-Sensitized Solar Cells with (001)-Oriented Anatase TiO2 Nanosheets Photoanode.

Project description:CdS/CdSe quantum dot-sensitized solar cells (QDSSCs) were fabricated on two types of TiO2 photoanodes, namely nanosheets (NSs) and nanoparticles. The TiO2 NSs with high (001)-exposed facets were prepared via a hydrothermal method, while the TiO2 nanoparticles used the commercial Degussa P-25. It was found that the pore size, specific surface area, porosity, and electron transport properties of TiO2 NSs were generally superior to those of P-25. As a result, the TiO2 NS-based CdS/CdSe QDSSC has exhibited a power conversion efficiency of 4.42%, which corresponds to a 54% improvement in comparison with the P-25-based reference cell. This study provides an effective photoanode design using nanostructure approach to improve the performance of TiO2-based QDSSCs.

| S-EPMC6329687 | biostudies-other

Electrochemical Properties of Carbon Aerogel Electrodes: Dependence on Synthesis Temperature.

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| S-EPMC6864835 | biostudies-literature

Revealing the Correlation of the Electrochemical Properties and the Hydration of Inkjet-Printed CdSe/CdS Semiconductor Gels.

Project description:The mobility of charge carriers across a semiconductor-nanoparticle-based 3D network (i.e., a gel) and the interfacial transfer of the charge carriers across the nanoparticle network/electrolyte boundary are elementary processes for applications in the fields of sensing and energy harvesting. The automated manufacturing of electrodes coated with porous networks can be realized by inkjet printing. By simultaneous printing of CdSe/CdS dot-in-rod-shaped nanorods (NRs) and the destabilization reagent, CdSe/CdS gel-network-coated electrodes can be obtained. In this work, the charge carrier mobility of the electrons and the holes within the porous CdSe/CdS nanorod gel network is investigated via photoelectrochemistry. Using linear sweep voltammograms (LSVs) and intensity-modulated photocurrent spectroscopy (IMPS), it is shown that the electron is moving within the tip-to-tip-connected CdSe/CdS NR gel structure, while the holes are trapped in the CdSe seed of the semiconductor heterostructures. Furthermore, the preparation process of gel structures is related to the elementary mechanism of hydration, which can be shown via photoelectrochemical long-term studies.

| S-EPMC7203843 | biostudies-literature

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