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1.
ACS Appl Mater Interfaces ; 13(38): 45600-45608, 2021 Sep 29.
Artículo en Inglés | MEDLINE | ID: mdl-34519472

RESUMEN

We report the design, fabrication, and characterization of silicon heterojunction microcells, a new type of photovoltaic cell that leverages high-efficiency bulk wafers in a microscale form factor, while also addressing the challenge of passivating microcell sidewalls to mitigate carrier recombination. We present synthesis methods exploiting either dry etching or laser cutting to realize microcells with native oxide-based edge passivation. Measured microcell performance for both fabrication processes is compared to that in simulations. We characterize the dependence of microcell open-circuit voltage (Voc) on the cell area-perimeter ratio and examine synthesis processes that affect edge passivation quality, such as sidewall damage removal, the passivation material, and the deposition technique. We report the highest Si microcell Voc to date (588 mV, for a 400 µm × 400 µm × 80 µm device), demonstrate Voc improvements with deposited edge passivation of up to 55 mV, and outline a pathway to achieve microcell efficiencies surpassing 15% for such device sizes.

2.
Adv Funct Mater ; 31(14)2021 Apr 01.
Artículo en Inglés | MEDLINE | ID: mdl-34305503

RESUMEN

Electrically conductive 3D periodic microscaffolds are fabricated using a particle-free direct ink writing approach for use as neuronal growth and electrophysiological recording platforms. A poly (2-hydroxyethyl methacrylate) (pHEMA)/pyrrole ink, followed by chemical in situ polymerization of pyrrole, enables hydrogel printing through nozzles as small as 1 µm. These conductive hydrogels can pattern complex 2D and 3D structures and have good biocompatibility with test cell cultures (~94.5% viability after 7 days). Hydrogel arrays promote extensive neurite outgrowth of cultured Aplysia californica pedal ganglion neurons. This platform allows extracellular electrophysiological recording of steady-state and stimulated electrical neuronal activities. In summation, this 3D conductive ink printing process enables preparation of biocompatible and micron-sized structures to create customized in vitro electrophysiological recording platforms.

3.
Nat Commun ; 12(1): 914, 2021 Feb 10.
Artículo en Inglés | MEDLINE | ID: mdl-33568629

RESUMEN

Oxide-supported noble metal catalysts have been extensively studied for decades for the water gas shift (WGS) reaction, a catalytic transformation central to a host of large volume processes that variously utilize or produce hydrogen. There remains considerable uncertainty as to how the specific features of the active metal-support interfacial bonding-perhaps most importantly the temporal dynamic changes occurring therein-serve to enable high activity and selectivity. Here we report the dynamic characteristics of a Pt/CeO2 system at the atomic level for the WGS reaction and specifically reveal the synergistic effects of metal-support bonding at the perimeter region. We find that the perimeter Pt0 - O vacancy-Ce3+ sites are formed in the active structure, transformed at working temperatures and their appearance regulates the adsorbate behaviors. We find that the dynamic nature of this site is a key mechanistic step for the WGS reaction.

4.
Nano Lett ; 20(4): 2620-2624, 2020 04 08.
Artículo en Inglés | MEDLINE | ID: mdl-32134671

RESUMEN

Cyclic voltammetry is demonstrated as a useful method to model equilibrium binding between quantum dots and redox active small molecules. Specifically, the interaction of a library of ferrocene derivatives with CdSe quantum dots is examined. For the strongly interacting systems, ferrocene carboxylic acid (FcCOOH) and ferrocene hexanethiol (Fc-hexSH), the binding equilibria can be quantitatively deduced by modeling the cyclic voltammetry data. This modeling allows extraction of the diffusion coefficients, equilibrium constants associated with both the reduced and oxidized species, and forward and reverse rates associated with binding for both the reduced and oxidized species. Taken together these data give direct insight into the binding of small molecules to quantum-dot surfaces as a function of oxidation state, critical information for the design of quantum dots as photoredox catalysts and charge transfer mediators.

5.
J Chem Phys ; 151(19): 194702, 2019 Nov 21.
Artículo en Inglés | MEDLINE | ID: mdl-31757130

RESUMEN

As the commercial display market grows, the demand for low-toxicity, highly emissive, and size-tunable semiconducting nanoparticles has increased. Indium phosphide quantum dots represent a promising solution to these challenges; unfortunately, they typically suffer from low inherent emissivity resulting from charge carrier trapping. Strategies to improve the emissive characteristics of indium phosphide often involve zinc incorporation into or onto the core itself and the fabrication of core/shell heterostructures. InP clusters are high fidelity platforms for studying processes such as cation exchange and surface doping with exogenous ions since these clusters are used as single-source precursors for quantum dot synthesis. Here, we examined the incorporation of zinc and gallium ions in InP clusters and the use of the resultant doped clusters as single-source precursors to emissive heterostructured nanoparticles. Zinc ions were observed to readily react with InP clusters, resulting in partial cation exchange, whereas gallium resisted cluster incorporation. Zinc-doped clusters effectively converted to emissive nanoparticles, with quantum yields strongly correlated with zinc content. On the other hand, gallium-doped clusters failed to demonstrate improvements in quantum dot emission. These results indicate stark differences in the mechanisms associated with aliovalent and isovalent doping and provide insight into the use of doped clusters to make emissive quantum dots.

6.
Chem Commun (Camb) ; 54(52): 7109-7122, 2018 Jun 26.
Artículo en Inglés | MEDLINE | ID: mdl-29872794

RESUMEN

The field of colloidal nanocrystal synthesis has progressed rapidly to the point where spherical colloids of diverse sizes and compositions are commercially available or can be synthesized with minimal synthetic training. As quantum dots work their way into a greater array of technologies, it has become increasingly important to maximize the uniformity of these nanoscale structures and the efficiency of associated photophysical processes. Anisotropic quantum nanocrystals and quantum confined heterostructures offer even greater customization and tunability of specific electronic and photonic properties compared to their spherical counterparts. However, synthetic access to these more advanced structures is less well understood, and existing synthetic approaches are often challenging to execute or replicate. This feature article provides an account of the various bottom-up and top-down methods that have been developed to prepare more complex quantum confined structures and highlights the progress that has been made in the preparation of colloidal semiconductor nanocrystal heterostructures. From this survey of existing methods, it becomes clear that seeded assembly of heterostructure architectures combines many of the advantages of both bottom-up and top-down approaches to enable the greatest potential control over a diversity of new, customizable heterostructures with added functionality.

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