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1.
Small ; 19(47): e2304057, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37491772

RESUMO

Herein, we report the design and synthesis of a layered redox-active, antiferromagnetic metal organic semiconductor crystals with the chemical formula [Cu(H2 O)2 V(µ-O)(PPA)2 ] (where PPA is phenylphosphonate). The crystal structure of [Cu(H2 O)2 V(µ-O)(PPA)2 ] shows that the metal phosphonate layers are separated by phenyl groups of the phenyl phosphonate linker. Tauc plotting of diffuse reflectance spectra indicates that [Cu(H2 O)2 V(µ-O)(PPA)2 ] has an indirect band gap of 2.19 eV. Photoluminescence (PL) spectra indicate a complex landscape of energy states with PL peaks at 1.8 and 2.2 eV. [Cu(H2 O)2 V(µ-O)(PPA)2 ] has estimated hybrid ionic and electronic conductivity values between 0.13 and 0.6 S m-1 . Temperature-dependent magnetization measurements show that [Cu(H2 O)2 V(µ-O)(PPA)2 ] exhibits short range antiferromagnetic order between Cu(II) and V(IV) ions. [Cu(H2 O)2 V(µ-O)(PPA)2 ] is also photoluminescent with photoluminescence quantum yield of 0.02%. [Cu(H2 O)2 V(µ-O)(PPA)2 ] shows high electrochemical, and thermal stability.

2.
Opt Express ; 31(12): 19428-19442, 2023 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-37381358

RESUMO

Perovskite-silicon tandem solar cells have made rapid progress in the last decade. Still, they suffer from multiple loss channels, one of them being optical losses including reflection and thermalization. In this study, the effect of structures at the air-perovskite and perovskite-silicon interface of the tandem solar cell stack on these two loss channels are evaluated. Regarding reflectance, every structure evaluated led to a reduction relative to the optimized planar stack. The best combination of structures evaluated reduced the reflection loss from 3.1 mA/cm2 (planar reference) to 1.0 mA/cm2 equivalent current. Additionally, nanostructured interfaces can lead to a reduction in thermalization losses by enhancing the absorptance in the perovskite sub-cell close to the bandgap. This means that more current can be generated at a higher voltage under the assumption that current-matching is maintained and the perovskite bandgap is increased accordingly, pathing the way towards higher efficiencies. Here, the largest benefit was obtained using a structure at the upper interface. The best result yielded an increase of 4.9%rel in efficiency. A comparison to a tandem solar cell using a fully textured approach with random pyramids on silicon shows potential benefits for the suggested nanostructured approach regarding thermalization losses, while reflectance is reduced at a similar level. In addition, the applicability of the concept in the module context is shown.

4.
Opt Express ; 30(21): 37957-37970, 2022 Oct 10.
Artigo em Inglês | MEDLINE | ID: mdl-36258374

RESUMO

Evaporated charge extraction layers from organic molecular materials are vital in perovskite-based solar cells. For opto-electronic device optimization their complex refractive indices must be known for the visible and near infrared wavelength regime; however, accurate determination from thin organic films below 50 nm can be challenging. By combining spectrophotometry, variable angle spectroscopic ellipsometry, and X-ray reflectivity with an algorithm that simultaneously fits all available spectra, the complex refractive index of evaporated Spiro-TTB and C60 layers is determined with high accuracy. Based on that, an optical losses analysis for perovskite silicon solar cells shows that 15 nm of Spiro-TTB in the front of a n-i-p device reduces current by only 0.1 mA/cm2, compared to a substantial loss of 0.5 mA/cm2 due to 15 nm of C60 in a p-i-n device. Optical device simulation predicts high optical generation current densities of 19.7 and 20.1 mA/cm2 for the fully-textured, module-integrated p-i-n and n-i-p devices, respectively.

5.
Nat Commun ; 12(1): 104, 2021 Jan 04.
Artigo em Inglês | MEDLINE | ID: mdl-33397918

RESUMO

Photonic structures can be designed to tailor luminescence properties of materials, which becomes particularly interesting for non-linear phenomena, such as photon upconversion. However, there is no adequate theoretical framework to optimize photonic structure designs for upconversion enhancement. Here, we present a comprehensive theoretical model describing photonic effects on upconversion and confirm the model's predictions by experimental realization of 1D-photonic upconverter devices with large statistics and parameter scans. The measured upconversion photoluminescence enhancement reaches 82 ± 24% of the simulated enhancement, in the mean of 2480 separate measurements, scanning the irradiance and the excitation wavelength on 40 different sample designs. Additionally, the trends expected from the modeled interaction of photonic energy density enhancement, local density of optical states and internal upconversion dynamics, are clearly validated in all experimentally performed parameter scans. Our simulation tool now opens the possibility of precisely designing photonic structure designs for various upconverting materials and applications.

6.
ACS Appl Mater Interfaces ; 12(5): 6496-6502, 2020 Feb 05.
Artigo em Inglês | MEDLINE | ID: mdl-31931567

RESUMO

Homogeneous layer formation on textured silicon substrates is essential for the fabrication of highly efficient monolithic perovskite silicon tandem solar cells. From all well-known techniques for the fabrication of perovskite solar cells (PSCs), the evaporation method offers the highest degree of freedom for layer-by-layer deposition independent of the substrate's roughness or texturing. Hole-transporting polymers with high hole mobility and structural stability have been used as effective hole-transporting materials (HTMs) of PSCs. However, the strong intermolecular interactions of the polymers do not allow for a layer formation via the evaporation method, which is a big challenge for the perovskite community. Herein, we first applied a hole-transporting terthiophene polymer (PTTh) as an HTM for evaporated PSCs via an in situ vapor-phase polymerization using iodine (I2) as a sublimable oxidative agent. PTTh showed high hole mobility of 1.2 × 10-3 cm2/(V s) and appropriate energy levels as HTM in PSCs (EHOMO = -5.3 eV and ELUMO = -3.3 eV). The PSCs with the in situ vapor-phase polymerized PTTh hole-transporting layer and a co-evaporated perovskite layer exhibited a photovoltaic conversion efficiency of 5.9%, as a proof of concept, and high cell stability over time. Additionally, the polymer layer could fully cover the pyramidal structure of textured silicon substrates and was identified as an effective hole-transporting material for perovskite silicon tandem solar cells by optical simulation.

7.
ACS Appl Mater Interfaces ; 11(49): 45796-45804, 2019 Dec 11.
Artigo em Inglês | MEDLINE | ID: mdl-31774645

RESUMO

Perovskite silicon tandem solar cells have the potential to overcome the efficiency limit of single-junction solar cells. For both monolithic and mechanically stacked tandem devices, a semi-transparent perovskite top solar cell, including a transparent contact, is required. Usually, this contact consists of a metal oxide buffer layer and a sputtered transparent conductive oxide. In this work, semi-transparent perovskite solar cells in the regular n-i-p structure are presented with tin-doped indium oxide (ITO) directly sputtered on the hole conducting material Spiro-OMeTAD. ITO process parameters such as sputter power, temperature, and pressure in the chamber are systematically varied. While a low temperature of 50 °C is crucial for good device performance, a low sputter power has only a slight effect, and an increased chamber pressure has no influence on device performance. For the 5 × 5 mm2 perovskite cell with a planar front side, a 105 nm thick ITO layer with a sheet resistance of 44 Ω sq-1 allowing for the omission of grid fingers and a MgF2 antireflection coating are used to improve transmission into the solar cells. The best device achieved an efficiency of 14.8%, which would result in 24.2% in a four-terminal tandem configuration.

9.
ACS Appl Mater Interfaces ; 11(1): 722-729, 2019 Jan 09.
Artigo em Inglês | MEDLINE | ID: mdl-30511836

RESUMO

Perovskite solar cells have become a game changer in the field of photovoltaics by reaching power conversion efficiencies beyond 23%. To achieve even higher efficiencies, it is necessary to increase the understanding of crystallization, grain formation, and layer ripening. In this study, by a systematic variation of methylammonium iodide (MAI) concentrations, we changed the stoichiometry and thereupon the crystal growth conditions in MAPbI3 perovskite solar cells, prepared by a two-step hybrid evaporation-spin-coating deposition method. Utilizing X-ray diffraction, scanning electron microscopy, atomic force microscopy, photoluminescence, and current-voltage ( J- V) characterization, we found that a relatively lower concentration of MAI, or in other words higher content of remnant and unconverted PbI2, correlates with smaller and stronger interconnected grains, as well as with an improved optoelectronic performance of the solar cells and mitigation of hysteresis. The possible explanations are grain and interface passivation by the excess PbI2 and a positive contribution of the grain boundaries to current extraction.

10.
Opt Express ; 26(18): A761-A768, 2018 Sep 03.
Artigo em Inglês | MEDLINE | ID: mdl-30184835

RESUMO

Silicon-based tandem solar cells and modules are complex systems that require optical modeling for the optimization towards highest efficiencies. The fact that such devices typically incorporate surface structures of different optical regimes poses high requirements to the involved simulation tools. The OPTOS formalism is ideally suited to deal with such complexity. Within this work OPTOS is extended in order to calculate the layer resolved absorptance in silicon-based tandem solar cells and module stacks. After describing the relevant mathematical details, a good agreement between OPTOS absorptance simulation results and EQE measurements of the current 33.3% record efficiency III-V on silicon two-terminal tandem solar cell is found. Furthermore, a detailed loss analysis is performed for an exemplary perovskite silicon solar cell with and without module encapsulation. The comparison reveals a lower photocurrent density for the module stack due to increased reflectance and absorption in the EVA.

11.
ACS Appl Mater Interfaces ; 10(31): 26293-26302, 2018 Aug 08.
Artigo em Inglês | MEDLINE | ID: mdl-30016061

RESUMO

Dual-source vapor-phase deposition enables low-temperature fabrication of high-performance planar structure perovskite (CH3NH3PbI3) solar cells (PSCs), applicable in tandem devices or for industrial production with high homogeneity. Herein, we report low-temperature fabrication of high-efficiency PSCs by dual-source vapor-phase deposition and significance of TiO2 surface modification with [6,6]-phenyl C61 butyric acid methyl ester (PCBM) on cell performance. Co-evaporation of PbI2 and CH3NH3I, as confirmed by X-ray diffraction and high-resolution transmission electron microscopy analyses, results in CH3NH3PbI3 layers with a well-crystallized tetragonal phase formed on both TiO2 and TiO2/PCBM electron-transport layers (ETLs). The devices with PCBM interlayer between TiO2 and CH3NH3PbI3 showed remarkably higher performance than those with TiO2 only, which was attributed to enhance charge extraction and reduced recombination at the TiO2/PCBM/CH3NH3PbI3 interface. The devices composed of evaporated CH3NH3PbI3 on top of the TiO2/PCBM and [2,2',7,7'-tetrakis( N, N-di- p-methoxyphenyl-amine)-9,9'-spirobifluorene] (Spiro-OMeTAD) as hole-transport material demonstrated power conversion efficiencies of 17.1% (reverse scan) and 13.4% (forward scan) with stabilized efficiency of over 16%, which is, to the best of our knowledge, the highest efficiency reported for evaporated perovskite solar cells using low-temperature fabrication method involving compact TiO2 layer as ETL. Furthermore, we show that this process can be used to deposit a CH3NH3PbI3 layer on top of a textured silicon substrate, which is the first step for preparing perovskite-silicon tandem devices with enhanced antireflection and light-trapping properties.

12.
Opt Express ; 26(6): 7537-7554, 2018 Mar 19.
Artigo em Inglês | MEDLINE | ID: mdl-29609308

RESUMO

This paper presents a simulation-based assessment of the potential for improving the upconversion efficiency of ß-NaYF4:Er3+ by embedding the upconverter in a one-dimensional photonic crystal. The considered family of structures consists of alternating quarter-wave layers of the upconverter material and a spacer material with a higher refractive index. The two photonic effects of the structures, a modified local energy density and a modified local density of optical states, are considered within a rate-equation-modeling framework, which describes the internal dynamics of the upconversion process. Optimal designs are identified, while taking into account production tolerances via Monte Carlo simulations. To determine the maximum upconversion efficiency across all realistically attainable structures, the refractive index of the spacer material is varied within the range of existing materials. Assuming a production tolerance of σ = 1 nm, the optimized structures enable more than 300-fold upconversion photoluminescence enhancements under one sun and upconversion quantum yields exceeding 15% under 30 suns concentration.

13.
Nat Mater ; 17(3): 218-219, 2018 03.
Artigo em Inglês | MEDLINE | ID: mdl-29358643
14.
ACS Appl Mater Interfaces ; 9(36): 30567-30574, 2017 Sep 13.
Artigo em Inglês | MEDLINE | ID: mdl-28834429

RESUMO

The most efficient organic-inorganic perovskite solar cells (PSCs) contain the conventional n-i-p mesoscopic device architecture using a semiconducting TiO2 scaffold combined with a compact TiO2 blocking layer for selective electron transport. These devices achieve high power conversion efficiencies (15-22%) but mainly require high-temperature sintering (>450 °C), which is not possible for temperature-sensitive substrates. Thus far, comparably little effort has been spent on alternative low-temperature (<150 °C) routes to realize high-efficiency TiO2-based PSCs; instead, other device architectures have been promoted for low-temperature processing. In this paper the compatibility of the conventional mesoscopic TiO2 device architecture with low-temperature processing is presented for the first time with the combination of electron beam evaporation for the compact TiO2 and UV treatment for the mesoporous TiO2 layer. Vacuum evaporation is introduced as an excellent deposition technique of uniform compact TiO2 layers, adapting smoothly to the rough fluorine-doped tin oxide substrate surface. Effective removal of organic binders by UV light is shown for the mesoporous scaffold. Entirely low-temperature-processed PSCs with TiO2 scaffold reach encouraging stabilized efficiencies of up to 18.2%. This process fulfills all requirements for monolithic tandem devices with high-efficiency silicon heterojunction solar cells as the bottom cell.

15.
Opt Express ; 24(13): 14895-914, 2016 Jun 27.
Artigo em Inglês | MEDLINE | ID: mdl-27410641

RESUMO

In this paper, we present a comprehensive simulation-based analysis of the two photonic effects of a Bragg stack - a modified local density of photon states (LDOS) and an enhanced local irradiance - on the upconversion (UC) luminescence and quantum yield of the upconverter ß-NaYF4 doped with 25% Er3+. The investigated Bragg stack consists of alternating layers of TiO2 and Poly(methylmethacrylate), the latter containing upconverter nanoparticles. Using experimentally determined input parameters, the photonic effects are first simulated separately and subsequently coupled in a rate equation model, describing the dynamics of the UC processes within ß-NaYF4:25% Er3+. With this integrated simulation model, the Bragg stack design is optimized to maximize either the UC quantum yield (UCQY) or UC luminescence. We find that in an optimized Bragg stack, due to the modified LDOS, the maximum UCQY is enhanced from 14% to 16%, compared to an unstructured layer of upconverter material. Additionally, this maximum UCQY can already be reached at an incident irradiance as low as 100 W/m2. With a Bragg stack design that maximizes UC luminescence, enhancement factors of up to 480 of the UC luminescence can be reached.

16.
Opt Express ; 24(14): A1083-93, 2016 Jul 11.
Artigo em Inglês | MEDLINE | ID: mdl-27410896

RESUMO

The OPTOS formalism is a matrix-based approach to determine the optical properties of textured optical sheets. It is extended within this work to enable the modelling of systems with an arbitrary number of textured, plane-parallel interfaces. A matrix-based system description is derived that accounts for the optical reflection and transmission interaction between all textured interfaces. Using OPTOS, we calculate reflectance and absorptance of complete photovoltaic module stacks, which consist of encapsulated silicon solar cells featuring textures that operate in different optical regimes. As exemplary systems, solar cells with and without module encapsulation are shown to exhibit a considerable absorptance gain if the random pyramid front side texture is combined with a diffractive rear side grating. A variation of the sunlight's angle of incidence reveals that the grating gain is almost not affected for incoming polar angles up to 60°. Considering as well the good agreement with alternative simulation techniques, OPTOS is demonstrated to be a versatile and efficient method for the optical analysis of photovoltaic modules.

17.
Opt Express ; 24(6): A434-45, 2016 Mar 21.
Artigo em Inglês | MEDLINE | ID: mdl-27136865

RESUMO

Due to their low reflectivity and effective light trapping properties black silicon nanostructured surfaces are promising front side structures for thin crystalline silicon solar cells. For further optimization of the light trapping effect, particularly in combination with rear side structures, it is necessary to simulate the optical properties of black silicon. Especially, the angular distribution of light in the silicon bulk after passage through the front side structure is relevant. In this paper, a rigorous coupled wave analysis of black silicon is presented, where the black silicon needle shaped structure is approximated by a randomized cone structure. The simulated absorptance agrees well with measurement data. Furthermore, the simulated angular light distribution within the silicon bulk shows that about 70% of the light can be subjected to internal reflection, highlighting the good light trapping properties.

18.
Opt Express ; 24(6): A460-75, 2016 Mar 21.
Artigo em Inglês | MEDLINE | ID: mdl-27136867

RESUMO

Photon upconversion is promising for many applications. However, the potential of lanthanide doped upconverter materials is typically limited by low absorption coefficients and low upconversion quantum yields (UCQY) under practical irradiance of the excitation. Modifying the photonic environment can strongly enhance the spontaneous emission and therefore also the upconversion luminescence. Additionally, the non-linear nature of the upconversion processes can be exploited by an increased local optical field introduced by photonic or plasmonic structures. In combination, both processes may lead to a strong enhancement of the UCQY at simultaneously lower incident irradiances. Here, we use a comprehensive 3D computation-based approach to investigate how absorption, upconversion luminescence, and UCQY of an upconverter are altered in the vicinity of spherical gold nanoparticles (GNPs). We use Mie theory and electrodynamic theory to compute the properties of GNPs. The parameters obtained in these calculations were used as input parameters in a rate equation model of the upconverter ß-NaYF4: 20% Er3+. We consider different diameters of the GNP and determine the behavior of the system as a function of the incident irradiance. Whether the UCQY is increased or actually decreased depends heavily on the position of the upconverter in respect to the GNP. Whereas the upconversion luminescence enhancement reaches a maximum around a distance of 35 nm to the surface of the GNP, we observe strong quenching of the UCQY for distances <40 nm and a UCQY maximum around 125 to 150 nm, in the case of a 300 nm diameter GNP. Hence, the upconverter material needs to be placed at different positions, depending on whether absorption, upconversion luminescence, or UCQY should be maximized. At the optimum position, we determine a maximum UCQY enhancement of 117% for a 300 nm diameter GNP at a low incident irradiance of 0.01 W/cm2. As the irradiance increases, the maximum UCQY enhancement decreases to 20% at 1 W/cm2. However, this UCQY enhancement translates into a significant improvement of the UCQY from 12.0% to 14.4% absolute.

19.
Opt Express ; 23(24): A1720-34, 2015 Nov 30.
Artigo em Inglês | MEDLINE | ID: mdl-26698818

RESUMO

In this paper we introduce the three-dimensional formulation of the OPTOS formalism, a matrix-based method that allows for the efficient simulation of non-coherent light propagation and absorption in thick textured sheets. As application examples, we calculate the absorptance of solar cells featuring textures on front and rear side with different feature sizes operating in different optical regimes. A discretization of polar and azimuth angle enables a three-dimensional description of systems with arbitrary surface textures. We present redistribution matrices for 3D surface textures, including pyramidal textures, binary crossed gratings and a Lambertian scatterer. The results of the OPTOS simulations for silicon sheets with different combinations of these surfaces are in accordance with both optical measurements and results based on established simulation methods like ray tracing. Using OPTOS, we show that the integration of a diffractive grating at the rear side of a silicon solar cell featuring a pyramidal front side results in absorption close to the Yablonovitch Limit enhancing the photocurrent density by 0.6 mA/cm2 for a 200 µm thick cell.

20.
Opt Express ; 23(11): A502-18, 2015 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-26072875

RESUMO

In this paper, we introduce a simulation formalism for determining the Optical Properties of Textured Optical Sheets (OPTOS). Our matrix-based method allows for the computationally-efficient calculation of non-coherent light propagation and absorption in thick textured sheets, especially solar cells, featuring different textures on front and rear side that may operate in different optical regimes. Within the simulated system, the angular power distribution is represented by a vector. This light distribution is modified by interaction with the surfaces of the textured sheets, which are described by redistribution matrices. These matrices can be calculated for each individual surface texture with the most appropriate technique. Depending on the feature size of the texture, for example, either ray- or wave-optical methods can be used. The comparison of the simulated absorption in a sheet of silicon for a variety of surface textures, both with the results from other simulation techniques and experimentally measured data, shows very good agreement. To demonstrate the versatility of this newly-developed approach, the absorption in silicon sheets with a large-scale structure (V-grooves) at the front side and a small-scale structure (diffraction grating) at the rear side is calculated. Moreover, with minimal computational effort, a thickness parameter variation is performed.

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