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1.
ACS Appl Mater Interfaces ; 16(36): 47931-47943, 2024 Sep 11.
Artículo en Inglés | MEDLINE | ID: mdl-39215382

RESUMEN

Full-area passivating contacts based on SiOx/poly-Si stacks are key for the new generation of industrial silicon solar cells substituting the passivated emitter and rear cell (PERC) technology. Demonstrating a potential efficiency increase of 1 to 2% compared to PERC, the utilization of n-type wafers with an n-type contact at the back and a p-type diffused boron emitter has become the industry standard in 2024. In this work, variations of this technology are explored, considering p-type passivating contacts on p-type Si wafers formed via a rapid thermal processing (RTP) step. These contacts could be useful in conjunction with n-type contacts for realizing solar cells with passivating contacts on both sides. Here, a particular focus is set on investigating the influence of the applied thermal treatment on the interfacial silicon oxide (SiOx) layer. Thin SiOx layers formed via ultraviolet (UV)-O3 exposure are compared with layers obtained through a plasma treatment with nitrous oxide (N2O). This process is performed in the same plasma enhanced chemical vapor deposition (PECVD) chamber used to grow the Si-based passivating layer, resulting in a streamlined process flow. For both oxide types, the influence of the RTP thermal budget on passivation quality and contact resistivity is investigated. Whereas the UV-O3 oxide shows a pronounced degradation when using high thermal budget annealing (T > 860 °C), the N2O-plasma oxide exhibits instead an excellent passivation quality under these conditions. Simultaneously, the contact resistivity achieved with the N2O-plasma oxide layer is comparable to that yielded by UV-O3-grown oxides. To unravel the mechanisms behind the improved performance obtained with the N2O-plasma oxide at high thermal budget, characterization by high-resolution (scanning) transmission electron microscopy (HR-(S)TEM), X-ray reflectometry (XRR) and X-ray photoelectron spectroscopy (XPS) is conducted on layer stacks featuring both N2O and UV-O3 oxides after RTP. A breakup of the UV-O3 oxide at high thermal budget is observed, whereas the N2O oxide is found to maintain its structural integrity along the interface. Furthermore, chemical analysis reveals that the N2O oxide is richer in oxygen and contains a higher amount of nitrogen compared to the UV-O3 oxide. These distinguishing characteristics can be directly linked to the enhanced stability exhibited by the N2O oxide under higher annealing temperatures and extended dwell times.

2.
ACS Appl Mater Interfaces ; 16(28): 36557-36566, 2024 Jul 17.
Artículo en Inglés | MEDLINE | ID: mdl-38949536

RESUMEN

Up-scalable coating processes need to be developed to manufacture efficient and stable perovskite-based solar modules. In this work, we combine two Lewis base additives (N,N'-dimethylpropyleneurea and thiourea) to fabricate high-quality Cs0.15FA0.85PbI3 perovskite films by blade-coating on large areas. Selected-area electron diffraction patterns reveal a minimization of stacking faults in the α-FAPbI3 phase for this specific cesium-formamidinium composition in both spin-coated and blade-coated perovskite films, demonstrating its scaling potential. The underlying mechanism of the crystallization process and the specific role of thiourea are characterized by Fourier transform infrared spectroscopy and in situ optical absorption, showing clear interaction between thiourea and perovskite precursors and halved film-formation activation energy (from 114 to 49 kJ/mol), which contribute to the obtained specific morphology with the formation of large domain sizes on a short time scale. The blade-coated perovskite solar cells demonstrate a maximum efficiency of approximately 16.9% on an aperture area of 1 cm2.

3.
Energy Environ Sci ; 17(11): 3832-3847, 2024 Jun 04.
Artículo en Inglés | MEDLINE | ID: mdl-38841317

RESUMEN

The technique of alloying FA+ with Cs+ is often used to promote structural stabilization of the desirable α-FAPbI3 phase in halide perovskite devices. However, the precise mechanisms by which these alloying approaches improve the optoelectronic quality and enhance the stability have remained elusive. In this study, we advance that understanding by investigating the effect of cationic alloying in CsxFA1-xPbI3 perovskite thin-films and solar-cell devices. Selected-area electron diffraction patterns combined with microwave conductivity measurements reveal that fine Cs+ tuning (Cs0.15FA0.85PbI3) leads to a minimization of stacking faults and an increase in the photoconductivity of the perovskite films. Ultra-sensitive external quantum efficiency, kelvin-probe force microscopy and photoluminescence quantum yield measurements demonstrate similar Urbach energy values, comparable surface potential fluctuations and marginal impact on radiative emission yields, respectively, irrespective of Cs content. Despite this, these nanoscopic defects appear to have a detrimental impact on inter-grains'/domains' carrier transport, as evidenced by conductive-atomic force microscopy and corroborated by drastically reduced solar cell performance. Importantly, encapsulated Cs0.15FA0.85PbI3 devices show robust operational stability retaining 85% of the initial steady-state power conversion efficiency for 1400 hours under continuous 1 sun illumination at 35 °C, in open-circuit conditions. Our findings provide nuance to the famous defect tolerance of halide perovskites while providing solid evidence about the detrimental impact of these subtle structural imperfections on the long-term operational stability.

4.
ACS Appl Nano Mater ; 7(6): 6242-6252, 2024 Mar 22.
Artículo en Inglés | MEDLINE | ID: mdl-38544504

RESUMEN

This work addresses the need for precise control of thin film sputtering processes to enable thin film material tailoring on the example of zinc tin nitride (ZTN) thin films deposited via microwave plasma-assisted high power reactive magnetron sputtering (MAR-HiPIMS). The applied in situ diagnostic techniques (Langmuir probe and energy-resolved time-of-flight mass spectrometry) supported monitoring changes in the deposition environment with respect to microwave (MW) power. During MAR-HiPIMS, the presence of nitride ions in the gas phase (ZnN+, ZnN2+, SnN+, SnN2+) was detected. This indicates that the MW plasma facilitated their production, as opposed to pure R-HiPIMS. Additionally, MW plasma caused post-ionisation of sputtered atoms and reduced the overall energy-per-charge range of incoming charged species. By varying the MW power and substrate biasing, films with comparable chemical compositions (approximately Zn0.92Sn1.08N2) but different structures, ranging from polycrystalline to preferentially textured, were successfully produced. The application of density functional theory (DFT) further enabled the relationship between the lattice parameters and the optical properties of ZTN to be explored, where the material's optical anisotropy nature was determined. It was found that despite considerable differences in crystallinity, the changes induced in the lattice parameters were subangstrom, causing only minor changes in the final optical properties of ZTN.

5.
Adv Mater ; 36(21): e2311745, 2024 May.
Artículo en Inglés | MEDLINE | ID: mdl-38300183

RESUMEN

The primary performance limitation in inverted perovskite-based solar cells is the interface between the fullerene-based electron transport layers and the perovskite. Atomic layer deposited thin aluminum oxide (AlOX) interlayers that reduce nonradiative recombination at the perovskite/C60 interface are developed, resulting in >60 millivolts improvement in open-circuit voltage and 1% absolute improvement in power conversion efficiency. Surface-sensitive characterizations indicate the presence of a thin, conformally deposited AlOx layer, functioning as a passivating contact. These interlayers work universally using different lead-halide-based absorbers with different compositions where the 1.55 electron volts bandgap single junction devices reach >23% power conversion efficiency. A reduction of metallic Pb0 is found and the compact layer prevents in- and egress of volatile species, synergistically improving the stability. AlOX-modified wide-bandgap perovskite absorbers as a top cell in a monolithic perovskite-silicon tandem enable a certified power conversion efficiency of 29.9% and open-circuit voltages above 1.92 volts for 1.17 square centimeters device area.

6.
J Phys Chem C Nanomater Interfaces ; 122(31): 17612-17620, 2018 Aug 09.
Artículo en Inglés | MEDLINE | ID: mdl-30258525

RESUMEN

Transparent conductive oxides (TCOs) are essential in technologies coupling light and electricity. For Sn-based TCOs, oxygen deficiencies and undercoordinated Sn atoms result in an extended density of states below the conduction band edge. Although shallow states provide free carriers necessary for electrical conductivity, deeper states inside the band gap are detrimental to transparency. In zinc tin oxide (ZTO), the overall optoelectronic properties can be improved by defect passivation via annealing at high temperatures. Yet, the high thermal budget associated with such treatment is incompatible with many applications. Here, we demonstrate an alternative, low-temperature passivation method, which relies on cosputtering Sn-based TCOs with silicon dioxide (SiO2). Using amorphous ZTO and amorphous/polycrystalline tin dioxide (SnO2) as representative cases, we demonstrate through optoelectronic characterization and density functional theory simulations that the SiO2 contribution is twofold. First, oxygen from SiO2 passivates the oxygen deficiencies that form deep defects in SnO2 and ZTO. Second, the ionization energy of the remaining deep defect centers is lowered by the presence of silicon atoms. Remarkably, we find that these ionized states do not contribute to sub-gap absorptance. This simple passivation scheme significantly improves the optical properties without affecting the electrical conductivity, hence overcoming the known transparency-conductivity trade-off in Sn-based TCOs.

7.
ACS Appl Mater Interfaces ; 9(8): 7241-7248, 2017 Mar 01.
Artículo en Inglés | MEDLINE | ID: mdl-28151638

RESUMEN

Two fundamental requirements of transparent conductive oxides are high conductivity and low optical absorptance, properties strongly dependent on the free-carrier concentration of the film. The free-carrier concentration is usually tuned by the addition of dopant atoms; which are commonly assumed to be uniformly distributed in the films or partially segregated at grain boundaries. Here, the combination of secondary ion mass spectroscopy at the nanometric scale (NanoSIMS) and Kelvin probe force microscopy (KPFM) allows direct imaging of boron-dopant distribution in polycrystalline zinc oxide (ZnO) films. This work demonstrates that the boron atoms have a bimodal spatial distribution within each grain of the ZnO films. NanoSIMS analysis shows that boron atoms are preferentially incorporated into one of the two sides of each ZnO grain. KPFM measurements confirm that boron atoms are electrically active, locally increasing the free-carrier concentration in the film. The proposed cause of this nonuniform dopant distribution is the different sticking coefficient of Zn adatoms on the two distinct surface terminations of the ZnO grains. The higher sticking coefficient of Zn on the c+ surface restricts the boron incorporation on this side of the grains, resulting in preferential boron incorporation on the c- side and causing the bimodal distribution.

8.
Nano Lett ; 16(11): 7013-7018, 2016 11 09.
Artículo en Inglés | MEDLINE | ID: mdl-27775887

RESUMEN

Changes in the nanostructure of methylammonium lead iodide (MAPbI3) perovskite solar cells are assessed as a function of current-voltage stimulus by biasing thin samples in situ in a transmission electron microscope. Various degradation pathways are identified both in situ and ex situ, predominantly at the positively biased MAPbI3 interface. Iodide migrates into the positively biased charge transport layer and also volatilizes along with organic species, which triggers the nucleation of PbI2 nanoparticles and voids and hence decreases the cell performance.

9.
Nano Lett ; 14(9): 5085-91, 2014 Sep 10.
Artículo en Inglés | MEDLINE | ID: mdl-25102168

RESUMEN

We demonstrate self-patterned insulating nanoparticle layers to define local electrical interconnects in thin-film electronic devices. We show this with thin-film silicon tandem solar cells, where we introduce between the two component cells a solution-processed SiO2 nanoparticle layer with local openings to allow for charge transport. Because of its low refractive index, high transparency, and smooth surface, the SiO2 nanoparticle layer acts as an excellent intermediate reflector allowing for efficient light management.

10.
Chem Commun (Camb) ; 50(15): 1808-10, 2014 Feb 21.
Artículo en Inglés | MEDLINE | ID: mdl-24400316

RESUMEN

Energy-filtered transmission electron microscopy images are acquired during the reduction of a NiO-YSZ composite in H2 up to 600 °C. Temperature-resolved quantitative information about both chemistry and structure is extracted with nm spatial resolution from the data, paving the way for the development of detailed reduction models.

11.
Adv Mater ; 24(9): 1182-6, 2012 Mar 02.
Artículo en Inglés | MEDLINE | ID: mdl-22290779

RESUMEN

Nanometer wide silicon filaments embedded in an amorphous silicon oxide matrix are grown at low temperatures over a large area. The optical and electrical properties of these mixed-phase nanomaterials can be tuned independently, allowing for advanced light management in high efficiency thin-film silicon solar cells and for band-gap tuning via quantum confinement in third-generation photovoltaics.


Asunto(s)
Luz , Nanoestructuras/química , Óxidos/química , Compuestos de Silicona/química , Silicio/química , Luminiscencia , Nanoestructuras/ultraestructura , Energía Solar
12.
Membranes (Basel) ; 2(3): 585-664, 2012 Aug 31.
Artículo en Inglés | MEDLINE | ID: mdl-24958298

RESUMEN

Solid oxide fuel cells are able to convert fuels, including hydrocarbons, to electricity with an unbeatable efficiency even for small systems. One of the main limitations for long-term utilization is the reduction-oxidation cycling (RedOx cycles) of the nickel-based anodes. This paper will review the effects and parameters influencing RedOx cycles of the Ni-ceramic anode. Second, solutions for RedOx instability are reviewed in the patent and open scientific literature. The solutions are described from the point of view of the system, stack design, cell design, new materials and microstructure optimization. Finally, a brief synthesis on RedOx cycling of Ni-based anode supports for standard and optimized microstructures is depicted.

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