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1.
Nanoscale ; 11(37): 17262-17269, 2019 Oct 07.
Artigo em Inglês | MEDLINE | ID: mdl-31246216

RESUMO

Perovskite nanoparticles have attracted the attention of research groups around the world for their impressive photophysical properties, facile synthesis and versatile surface chemistry. Here, we report a synthetic route that takes advantage of a suite of soluble precursors to generate CsPbBr3 perovskite nanoplatelets with fine control over size, thickness and optical properties. We demonstrate near unit cell precision, creating well characterized materials with sharp, narrow emission lines at 430, 460 and 490 nm corresponding to nanoplatelets that are 2, 4, and 6 unit cells thick, respectively. Nanoplatelets were characterized with optical spectroscopy, atomic force microscopy, scanning electron microscopy and transmission electron microscopy to explicitly correlate growth conditions, thickness and resulting photophysical properties. Detailed in situ photoluminescence spectroscopic studies were carried out to understand and optimize particle growth by correlating light emission with nanoplatelet growth across a range of synthetic conditions. It was found that nanoplatelet thickness and emission wavelength increase as the ratio of oleic acid to oleyl amine or the reaction temperature is increased. Using this information, we control the lateral size, width and corresponding emission wavelength of the desired nanoplatelets by modulating the temperature and ratios of the ligand.

2.
Nano Lett ; 18(6): 3473-3480, 2018 06 13.
Artigo em Inglês | MEDLINE | ID: mdl-29709191

RESUMO

Mixed cation metal halide perovskites with increased power conversion efficiency, negligible hysteresis, and improved long-term stability under illumination, moisture, and thermal stressing have emerged as promising compounds for photovoltaic and optoelectronic applications. Here, we shed light on photoinduced halide demixing using in situ photoluminescence spectroscopy and in situ synchrotron X-ray diffraction (XRD) to directly compare the evolution of composition and phase changes in CH(NH2)2CsPb-halide (FACsPb-) and CH3NH3Pb-halide (MAPb-) perovskites upon illumination, thereby providing insights into why FACs-perovskites are less prone to halide demixing than MA-perovskites. We find that halide demixing occurs in both materials. However, the I-rich domains formed during demixing accumulate strain in FACsPb-perovskites but readily relax in MA-perovskites. The accumulated strain energy is expected to act as a stabilizing force against halide demixing and may explain the higher Br composition threshold for demixing to occur in FACsPb-halides. In addition, we find that while halide demixing leads to a quenching of the high-energy photoluminescence emission from MA-perovskites, the emission is enhanced from FACs-perovskites. This behavior points to a reduction of nonradiative recombination centers in FACs-perovskites arising from the demixing process and buildup of strain. FACsPb-halide perovskites exhibit excellent intrinsic material properties with photoluminescence quantum yields that are comparable to MA-perovskites. Because improved stability is achieved without sacrificing electronic properties, these compositions are better candidates for photovoltaic applications, especially as wide bandgap absorbers in tandem cells.

3.
J Vis Exp ; (127)2017 09 08.
Artigo em Inglês | MEDLINE | ID: mdl-28930986

RESUMO

Organo-lead halide perovskites have recently attracted great interest for potential applications in thin-film photovoltaics and optoelectronics. Herein, we present a protocol for the fabrication of this material via the low-pressure vapor assisted solution process (LP-VASP) method, which yields ~19% power conversion efficiency in planar heterojunction perovskite solar cells. First, we report the synthesis of methylammonium iodide (CH3NH3I) and methylammonium bromide (CH3NH3Br) from methylamine and the corresponding halide acid (HI or HBr). Then, we describe the fabrication of pinhole-free, continuous methylammonium-lead halide perovskite (CH3NH3PbX3 with X = I, Br, Cl and their mixture) films with the LP-VASP. This process is based on two steps: i) spin-coating of a homogenous layer of lead halide precursor onto a substrate, and ii) conversion of this layer to CH3NH3PbI3-xBrx by exposing the substrate to vapors of a mixture of CH3NH3I and CH3NH3Br at reduced pressure and 120 °C. Through slow diffusion of the methylammonium halide vapor into the lead halide precursor, we achieve slow and controlled growth of a continuous, pinhole-free perovskite film. The LP-VASP allows synthetic access to the full halide composition space in CH3NH3PbI3-xBrx with 0 ≤ x ≤ 3. Depending on the composition of the vapor phase, the bandgap can be tuned between 1.6 eV ≤ Eg ≤ 2.3 eV. In addition, by varying the composition of the halide precursor and of the vapor phase, we can also obtain CH3NH3PbI3-xClx. Films obtained from the LP-VASP are reproducible, phase pure as confirmed by X-ray diffraction measurements, and show high photoluminescence quantum yield. The process does not require the use of a glovebox.


Assuntos
Compostos de Cálcio/química , Chumbo/química , Metilaminas/química , Óxidos/química , Titânio/química , Soluções , Pressão de Vapor
4.
Nat Commun ; 7: 12446, 2016 08 18.
Artigo em Inglês | MEDLINE | ID: mdl-27534585

RESUMO

Formation of planar heterojunction perovskite solar cells exhibiting both high efficiency and stability under continuous operation remains a challenge. Here, we show this can be achieved by using a defective TiO2 thin film as the electron transport layer. TiO2 layers with native defects are deposited by electron beam evaporation in an oxygen-deficient environment. Deep-level hole traps are introduced in the TiO2 layers and contribute to a high photoconductive gain and reduced photocatalytic activity. The high photoconductivity of the TiO2 electron transport layer leads to improved efficiency for the fabricated planar devices. A maximum power conversion efficiency of 19.0% and an average PCE of 17.5% are achieved. In addition, the reduced photocatalytic activity of the TiO2 layer leads to enhanced long-term stability for the planar devices. Under continuous operation near the maximum power point, an efficiency of over 15.4% is demonstrated for 100 h.

5.
Phys Chem Chem Phys ; 18(23): 15988-94, 2016 Jun 21.
Artigo em Inglês | MEDLINE | ID: mdl-27240735

RESUMO

Secondary phases zinc sulfide/selenide and copper sulfide in Cu2ZnSnS4 (CZTS) and Cu2ZnSnSe4 (CZTSe) thin film samples are investigated by X-ray absorption near edge structure (XANES) analysis at the chalcogen K-edges. Because of the formation of secondary phases the composition of the kesterite phase can deviate significantly from the total sample composition. For a large set of non-stoichiometric samples we find that the cation ratios of the kesterite phase never exceed Zn/Sn = 1 even for Zn-rich CZTS and CZTSe, with all excess Zn being contained in secondary phases. For CZTS the cation ratios are found to be additionally constrained by Cu/Sn ≤ 2, which means that Cu-excess always leads to the formation of CuxS secondary phases. These results give clear bounds on the Cu-rich and Zn-rich sides of the single phase region in polycrystalline CZTS/Se thin films.

6.
Nano Lett ; 16(7): 4047-53, 2016 07 13.
Artigo em Inglês | MEDLINE | ID: mdl-27322506

RESUMO

Molybdenum disulfide (MoS2) has been widely examined as a catalyst containing no precious metals for the hydrogen evolution reaction (HER); however, these examinations have utilized synthesized MoS2 because the pristine MoS2 mineral is known to be a poor catalyst. The fundamental challenge with pristine MoS2 is the inert HER activity of the predominant (0001) basal surface plane. In order to achieve high HER performance with pristine MoS2, it is essential to activate the basal plane. Here, we report a general thermal process in which the basal plane is texturized to increase the density of HER-active edge sites. This texturization is achieved through a simple thermal annealing procedure in a hydrogen environment, removing sulfur from the MoS2 surface to form edge sites. As a result, the process generates high HER catalytic performance in pristine MoS2 across various morphologies such as the bulk mineral, films composed of micron-scale flakes, and even films of a commercially available spray of nanoflake MoS2. The lowest overpotential (η) observed for these samples was η = 170 mV to obtain 10 mA/cm(2) of HER current density.

7.
Nat Commun ; 7: 10502, 2016 Jan 27.
Artigo em Inglês | MEDLINE | ID: mdl-26813257

RESUMO

The III-V compound semiconductors exhibit superb electronic and optoelectronic properties. Traditionally, closely lattice-matched epitaxial substrates have been required for the growth of high-quality single-crystal III-V thin films and patterned microstructures. To remove this materials constraint, here we introduce a growth mode that enables direct writing of single-crystalline III-V's on amorphous substrates, thus further expanding their utility for various applications. The process utilizes templated liquid-phase crystal growth that results in user-tunable, patterned micro and nanostructures of single-crystalline III-V's of up to tens of micrometres in lateral dimensions. InP is chosen as a model material system owing to its technological importance. The patterned InP single crystals are configured as high-performance transistors and photodetectors directly on amorphous SiO2 growth substrates, with performance matching state-of-the-art epitaxially grown devices. The work presents an important advance towards universal integration of III-V's on application-specific substrates by direct growth.

8.
Nano Lett ; 16(1): 800-6, 2016 Jan 13.
Artigo em Inglês | MEDLINE | ID: mdl-26691065

RESUMO

Hybrid organic-inorganic halide perovskite based semiconductor materials are attractive for use in a wide range of optoelectronic devices because they combine the advantages of suitable optoelectronic attributes and simultaneously low-cost solution processability. Here, we present a two-step low-pressure vapor-assisted solution process to grow high quality homogeneous CH3NH3PbI3-xBrx perovskite films over the full band gap range of 1.6-2.3 eV. Photoluminescence light-in versus light-out characterization techniques are used to provide new insights into the optoelectronic properties of Br-containing hybrid organic-inorganic perovskites as a function of optical carrier injection by employing pump-powers over a 6 orders of magnitude dynamic range. The internal luminescence quantum yield of wide band gap perovskites reaches impressive values up to 30%. This high quantum yield translates into substantial quasi-Fermi level splitting and high "luminescence or optically implied" open-circuit voltage. Most importantly, both attributes, high internal quantum yield and high optically implied open-circuit voltage, are demonstrated over the entire band gap range (1.6 eV ≤ Eg ≤ 2.3 eV). These results establish the versatility of Br-containing perovskite semiconductors for a variety of applications and especially for the use as high-quality top cell in tandem photovoltaic devices in combination with industry dominant Si bottom cells.

9.
Sci Rep ; 5: 16028, 2015 Nov 03.
Artigo em Inglês | MEDLINE | ID: mdl-26526426

RESUMO

The non-toxic and wide bandgap material TiO2 is explored as an n-type buffer layer on p-type Cu(In,Ga)Se2 (CIGS) absorber layer for thin film solar cells. The amorphous TiO2 thin film deposited by atomic layer deposition process at low temperatures shows conformal coverage on the CIGS absorber layer. Solar cells from non-vacuum deposited CIGS absorbers with TiO2 buffer layer result in a high short-circuit current density of 38.9 mA/cm(2) as compared to 36.9 mA/cm(2) measured in the reference cell with CdS buffer layer, without compromising open-circuit voltage. The significant photocurrent gain, mainly in the UV part of the spectrum, can be attributed to the low parasitic absorption loss in the ultrathin TiO2 layer (~10 nm) with a larger bandgap of 3.4 eV compared to 2.4 eV of the traditionally used CdS. Overall the solar cell conversion efficiency was improved from 9.5% to 9.9% by substituting the CdS by TiO2 on an active cell area of 10.5 mm(2). Optimized TiO2/CIGS solar cells show excellent long-term stability. The results imply that TiO2 is a promising buffer layer material for CIGS solar cells, avoiding the toxic CdS buffer layer with added performance advantage.

10.
J Phys Chem Lett ; 6(12): 2177-82, 2015 Jun 18.
Artigo em Inglês | MEDLINE | ID: mdl-26266588

RESUMO

To date, some of the highest performance photocathodes of a photoelectrochemical (PEC) cell have been shown with single-crystalline p-type InP wafers, exhibiting half-cell solar-to-hydrogen conversion efficiencies of over 14%. However, the high cost of single-crystalline InP wafers may present a challenge for future large-scale industrial deployment. Analogous to solar cells, a thin-film approach could address the cost challenges by utilizing the benefits of the InP material while decreasing the use of expensive materials and processes. Here, we demonstrate this approach, using the newly developed thin-film vapor-liquid-solid (TF-VLS) nonepitaxial growth method combined with an atomic-layer deposition protection process to create thin-film InP photocathodes with large grain size and high performance, in the first reported solar device configuration generated by materials grown with this technique. Current-voltage measurements show a photocurrent (29.4 mA/cm(2)) and onset potential (630 mV) approaching single-crystalline wafers and an overall power conversion efficiency of 11.6%, making TF-VLS InP a promising photocathode for scalable and efficient solar hydrogen generation.

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