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1.
ACS Appl Mater Interfaces ; 15(27): 32621-32628, 2023 Jul 12.
Artículo en Inglés | MEDLINE | ID: mdl-37368062

RESUMEN

Electron transport layers (ETL) based on tin(IV) oxide (SnO2) are recurrently employed in perovskite solar cells (PSCs) by many deposition techniques. Pulsed laser deposition (PLD) offers a few advantages for the fabrication of such layers, such as being compatible with large scale, patternable, and allowing deposition at fast rates. However, a precise understanding of how the deposition parameters can affect the SnO2 film, and as a consequence the solar cell performance, is needed. Herein, we use a PLD tool equipped with a droplet trap to minimize the number of excess particles (originated from debris) reaching the substrate, and we show how to control the PLD chamber pressure to obtain surfaces with very low roughness and how the concentration of oxygen in the background gas can affect the number of oxygen vacancies in the film. Using optimized deposition conditions, we obtained solar cells in the n-i-p configuration employing methylammonium lead iodide perovskite as the absorber layer with power conversion efficiencies exceeding 18% and identical performance to devices having the more typical atomic layer deposited SnO2 ETL.

2.
Energy Adv ; 1(5): 252-257, 2022 May 19.
Artículo en Inglés | MEDLINE | ID: mdl-35747761

RESUMEN

Vacuum processing is considered to be a promising method allowing the scalable fabrication of perovskite solar cells (PSCs). In vacuum processed PSCs, the n-i-p structure employing organic charge transport layers is less common than the p-i-n structure due to limited options to achieve an efficient electron extraction layer (EEL) on indium tin oxide (ITO) with vacuum thermal evaporation. There are a number of specific applications where an n-i-p structure is required and therefore, it is of interest to have alternative solutions for the n-type contact in vacuum processed PSCs. In this work, we report an efficient vacuum deposited EEL using a mixture of conventional organic small molecules, C60 and bathocuproine (BCP). Incorporation of BCP into C60 does not result in conventional n-doping; however, we observed enhanced charge extraction, which significantly increased the power conversion efficiency (PCE) from 13.1% to 18.1% in all-vacuum processed PSCs. The C60:BCP mixed (co-sublimated) film most likely results in shifted energy levels leading to better alignment with the electrodes.

3.
Adv Mater ; 31(39): e1902692, 2019 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-31420922

RESUMEN

Methylammonium lead triiodide (MAPI) has emerged as a high-performance photovoltaic material. Common understanding is that at room temperature, it adopts a tetragonal phase and it only converts to the perfect cubic phase around 50-60 °C. Most MAPI films are prepared using a solution-based coating process, yet they can also be obtained by vapor-phase deposition methods. Vapor-phase-processed MAPI films have significantly different characteristics than their solvent-processed analogous, such as relatively small crystal-grain sizes and short excited-state lifetimes. However, solar cells based on vapor-phase-processed MAPI films exhibit high power-conversion efficiencies. Surprisingly, after detailed characterization it is found that the vapor-phase-processed MAPI films adopt a cubic crystal structure at room temperature that is stable for weeks, even in ambient atmosphere. Furthermore, it is demonstrated that by tuning the deposition rates of both precursors during codeposition it is possible to vary the perovskite phase from cubic to tetragonal at room temperature. These findings challenge the common belief that MAPI is only stable in the tetragonal phase at room temperature.

4.
ACS Appl Mater Interfaces ; 11(26): 23320-23328, 2019 Jul 03.
Artículo en Inglés | MEDLINE | ID: mdl-31180209

RESUMEN

A variety of experiments on vacuum-deposited methylammonium lead iodide perovskite solar cells are presented, including JV curves with different scan rates, light intensity-dependent open-circuit voltage, impedance spectra, intensity-modulated photocurrent spectra, transient photocurrents, and transient voltage step responses. All these experimental data sets are successfully reproduced by a charge drift-diffusion simulation model incorporating mobile ions and charge traps using a single set of parameters. While previous modeling studies focused on a single experimental technique, we combine steady-state, transient, and frequency-domain simulations and measurements. Our study is an important step toward quantitative simulation of perovskite solar cells, leading to a deeper understanding of the physical effects in these materials. The analysis of the transient current upon voltage turn-on in the dark reveals that the charge injection properties of the interfaces are triggered by the accumulation of mobile ionic defects. We show that the current rise of voltage step experiments allow for conclusions about the recombination at the interface. Whether one or two mobile ionic species are used in the model has only a minor influence on the observed effects. A delayed current rise observed upon reversing the bias from +3 to -3 V in the dark cannot be reproduced yet by our drift-diffusion model. We speculate that a reversible chemical reaction of mobile ions with the contact material may be the cause of this effect, thus requiring a future model extension. A parameter variation is performed in order to understand the performance-limiting factors of the device under investigation.

5.
Front Chem ; 7: 936, 2019.
Artículo en Inglés | MEDLINE | ID: mdl-32039155

RESUMEN

Hole transport layers (HTLs) are of fundamental importance in perovskite solar cells (PSCs), as they must ensure an efficient and selective hole extraction, and ohmic charge transfer to the corresponding electrodes. In p-i-n solar cells, the ITO/HTL is usually not ohmic, and an additional interlayer such as MoO3 is usually placed in between the two materials by vacuum sublimation. In this work, we evaluated the properties of the MoO3/TaTm (TaTm is the HTL N4,N4,N4″,N4″-tetra([1,1'-biphenyl]-4-yl)-[1,1':4',1″-terphenyl]-4,4″-diamine) hole extraction interface by selectively annealing either MoO3 (prior to the deposition of TaTm) or the bilayer MoO3/TaTm (without pre-treatment on the MoO3), at temperature ranging from 60 to 200°C. We then used these p-contacts for the fabrication of a large batch of fully vacuum deposited PSCs, using methylammonium lead iodide as the active layer. We show that annealing the MoO3/TaTm bilayers at high temperature is crucial to obtain high rectification with low non-radiative recombination, due to an increase of the electrode work function and the formation of an ohmic interface with TaTm.

6.
J Phys Chem Lett ; 10(17): 5167-5172, 2019 Sep 05.
Artículo en Inglés | MEDLINE | ID: mdl-31423783

RESUMEN

It is widely accepted that a long photoluminescence (PL) lifetime in metal halide perovskite films is a crucial and favorable factor, as it ensures a large charge diffusion length leading to a high power conversion efficiency (PCE) in solar cells. It has been recently found that vacuum-evaporated CH3NH3PbI3 (eMAPI) films show very short PL lifetimes of several nanoseconds. The corresponding solar cells, however, have high photovoltage (>1.1 V) and PCEs (up to 20%). We rationalize this apparent contradiction and show that eMAPI films are characterized by a very high diffusion coefficient D, estimated from modeling the PL kinetics to exceed 1 cm2/s. Such high D values are favorable for long diffusion length as well as fast transport of carriers to film surfaces, where they recombine nonradiatively with surface recombination velocity S ∼ 104 cm/s. Possible physical origins leading to the high D values are also discussed.

7.
Dalton Trans ; 48(1): 30-34, 2018 Dec 18.
Artículo en Inglés | MEDLINE | ID: mdl-30431035

RESUMEN

Efficient perovskite devices consist of a perovskite film sandwiched between charge selective layers, in order to avoid non-radiative recombination. A common metal oxide used as a p-type or hole transport layer is molybdenum oxide. MoO3 is of particular interest for its very large work function, which allows it to be used both as an interfacial charge transfer material and a dopant for organic semiconductors. However, high quality and high work function MoO3 is typically thermally evaporated in a vacuum. An alternative solution-processable high work function material is phosphomolybdic acid (PMA), which is stable, commercially available and environmentally friendly. In this Communication, we show the first application of PMA in efficient vacuum processed perovskite devices. We found that the direct growth of perovskite films onto PMA leads to strong charge carrier recombination, hindering the solar cell photovoltage. Using an energetically suitable selective transport layer placed between PMA and the perovskite film, solar cells with efficiency >13% as well as LEDs with promising quantum efficiency can be obtained.

8.
J Phys Chem Lett ; 9(5): 1041-1046, 2018 Mar 01.
Artículo en Inglés | MEDLINE | ID: mdl-29432009

RESUMEN

Vacuum deposition is one of the most technologically relevant techniques for the fabrication of perovskite solar cells. The most efficient vacuum-based devices rely on doped organic contacts, compromising the long-term stability of the system. Here, we introduce an inorganic electron-transporting material to obtain power conversion efficiencies matching the best performing vacuum-deposited devices, with open-circuit potential close to the thermodynamic limit. We analyze the leakage current reduction and the interfacial recombination improvement upon use of a thin (<10 nm) interlayer of C60, as well as a more favorable band alignment after a bias/ultraviolet light activation process. This work presents an alternative for organic contacts in highly efficient vacuum-deposited perovskite solar cells.

9.
Adv Mater ; 28(44): 9839-9845, 2016 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-27717027

RESUMEN

The addition of Sr2+ in CH3 NH3 PbI3 perovskite films enhances the charge carrier collection efficiency of solar cells leading to very high fill factors, up to 85%. The charge carrier lifetime of Sr2+ -containing perovskites is in excess of 40 µs, longer than those reported for perovskite single crystals.

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