skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Rapid thermal annealing of CH 3 NH 3 PbI 3 perovskite thin films by intense pulsed light with aid of diiodomethane additive
The organic metal halide perovskite material is capable of high throughput manufacturing via traditional deposition processes used in roll-to-roll, yet thermal annealing post deposition may require long ovens. We report rapid annealed perovskite thin films using intense pulsed light (IPL) to initiate a radiative thermal response that is enabled by an alkyl halide additive that collectively improves the performance of a device processed in an ambient environment from a baseline of 10 to 16.5% efficiency. Previous reports on CH 3 NH 3 PbI 3 perovskite films using IPL processing achieved functional devices in milli-second time scales and are promising for high throughput manufacturing processes under ambient conditions. In this study, we found that the addition of diiodomethane (CH 2 I 2 ) as an additive to the methylammonium iodide (MAI)/lead iodide (PbI 2 ) precursor ink chemistry and subsequent IPL thermal annealing are inter-dependent. The concentration of CH 2 I 2 and IPL processing parameters have a direct effect on the surface morphology of the films and performance within a perovskite solar cell (PSC). The CH 2 I 2 dissociates under exposure to ultraviolet (UV) radiation from the IPL source liberating iodine ions in the film, influencing the perovskite formation and reducing the defect states. We anticipate that these results can be utilized to further develop different ink formulations using alkyl halides for the IPL technique to improve the performance of perovskite solar cells processed in ambient conditions.  more » « less
Award ID(s):
1828355
PAR ID:
10100869
Author(s) / Creator(s):
; ; ; ;
Date Published:
Journal Name:
Journal of Materials Chemistry A
Volume:
6
Issue:
20
ISSN:
2050-7488
Page Range / eLocation ID:
9378 to 9383
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Rapid advancements within photovoltaics realm necessitates swift fabrication of the modules using cheap materials through cost effective manufacturing processes to achieve short cost payback time. Photovoltaics manufacturing includes chemical processing of the materials followed by thermal annealing. Yet, long-term annealing of the materials using high temperature furnaces have remained the prevalent post-processing approach in industry which necessitates alternative methods to achieve high performance modules through rapid and economical processes. Intense pulse light (IPL) has been successfully applied as a promising rapid post-process annealing for various thin film photovoltaics, particularly to process the organic-inorganic perovskite solar cell (PSC) layers. In this paper, several results pertinent to the application of IPL on perovskite and SnO2 electron transport thin films are presented and the role of IPL on rapid thermal annealing (RTA) is explained. We show that swift fabrication of PSCs through IPL can result in efficiencies exceeding 16% when the Perovskite film is annealed with aid of CH2I2 alkyl halide additive in the ambient with 60% relative humidity. In addition, the synergy of IPL-alkyl halide interaction for other perovskite chemistries is introduced. We show that achieving to PSCs exceeding 12% efficiency was possible when the perovskite and SnO2 ETL was annealed sequentially through IPL. 
    more » « less
  2. Abstract The energy level alignment that occurs at the interfaces in planar-hetero structured perovskite photovoltaic devices strongly influences the charge transport across the interface, and thus plays a crucial role in overall device performance. To directly observe the energy level alignment requires pristine homogeneous surfaces that are free of contamination including adventitious carbon. Co-evaporation offers the ability to grow perovskite thin films in-situ, and the method involves thermally evaporating the perovskite precursors such as PbI 2 and CH 3 NH 3 I. Early reports have shown that the perovskite film formation and stoichiometry are problematic at ultralow coverages. In particular, it was reported that there was excessive PbI 2 and a deficiency in CH 3 NH 3 I. Using photoemission spectroscopy, we investigated the perovskite precursor PbI 2 on gold and highly oriented pyrolytic graphite (HOPG) surfaces. Results show that the nature of the surface and the deposition conditions can strongly influence the film formation. Excessive iodine observed in the initial evaporation stages appears to be substrate dependent, and this may influence the overall energy level alignment. 
    more » « less
  3. Abstract The performance of large‐area perovskite solar cells (PSCs) has been assessed for typical compositions, such as methylammonium lead iodide (MAPbI3), using a blade coater, slot‐die coater, solution shearing, ink‐jet printing, and thermal evaporation. However, the fabrication of large‐area all‐inorganic perovskite films is not well developed. This study develops, for the first time, an eco‐friendly solvent engineered all‐inorganic perovskite ink of dimethyl sulfoxide (DMSO) as a main solvent with the addition of acetonitrile (ACN), 2‐methoxyethanol (2‐ME), or a mixture of ACN and 2‐ME to fabricate large‐area CsPbI2.77Br0.23films with slot‐die coater at low temperatures (40–50 °C). The perovskite phase, morphology, defect density, and optoelectrical properties of prepared with different solvent ratios are thoroughly examined and they are correlated with their respective colloidal size distribution and solar cell performance. The optimized slot‐die‐coated CsPbI2.77Br0.23perovskite film, which is prepared from the eco‐friendly binary solvents dimethyl sulfoxide:acetonitrile (0.8:0.2 v/v), demonstrates an impressive power conversion efficiency (PCE) of 19.05%. Moreover, the device maintains ≈91% of its original PCE after 1 month at 20% relative humidity in the dark. It is believed that this study will accelerate the reliable manufacturing of perovskite devices. 
    more » « less
  4. While there has been rapid progress in the performance of perovskite solar cells, the details of film formation, effect of processing parameters and perovskite crystal structure are still under discussion. The details of the X-ray diffraction (XRD) pattern of the tetragonal phase of CH 3 NH 3 PbI 3 perovskite existing at room temperature are often overlooked, with unresolved (002) (at 2 θ = 13.99° for CuK α and q = 0.9927 Å −1 ) and (110) (at 2 θ = 14.14° and q = 1.003 Å −1 ) peaks considered to be one peak at 14°, leading to an inaccurate estimation of lattice parameters. In this study, we use an electrospray deposition technique to prepare perovskite films at room temperature, oriented in (002) and (110) directions, with (002) as the preferred orientation. The results of a detailed study on the emergence of the two orientations during perovskite formation are reported. The effect of process parameters, such as substrate temperature during deposition and annealing temperature, on the grain orientation was established using XRD and grazing incidence wide angle X-ray scattering (GIWAXS). The study suggests that an irreversible crystal reorientation from (002) to (110) occurs at high temperature during rapid annealing, whereas a reversible crystal thermal expansion is seen during slow annealing. Finally, the results of the grain reorientation are correlated with the film properties, and it is shown that the film with the dominant (110) orientation has improved morphology and optoelectronic properties. The detailed structural investigation and characterization presented in this study are important for the precise determination of crystal orientation and achievement of desirable photovoltaic properties of the absorber material by carefully observing the adjacent crystal plane peaks in the XRD pattern of the perovskite thin films. 
    more » « less
  5. Li, Gang; Nguyen, Thuc-Quyen; Nogueira, Ana Flávia; Rand, Barry P.; Moons, Ellen; Stingelin, Natalie (Ed.)
    Anti-solvent-free one-step deposition of perovskite thin film shows promising potential for application in slot-die or roll-to-roll mass fabrication processes of perovskite solar cells. The continuous coverage was confirmed by PV response of devices made using the on-step deposition process. In this work, we have developed a process to deposit MAPB0.75Sn0.25(I0.5Br0.5)3 perovskite thin films without anti-solvent adding MAAc to the ink. By varying the Br content of the perovskite precursor, we were able to tune the bandpap. Fabricated solar cells with the structure ITO/CuI/MAPb0.75Sn0.25(I0.5Br0.5)3/C60/BCP/Al with PCE of 4.59% show the parth of the fabrication process of antisolvent-free tin-lead-based solar cells. 
    more » « less