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Dimethylammonium Addition to Halide Perovskite Precursor Increases Vertical and Lateral Heterogeneity

Journal Article · · ACS Energy Letters
 [1];  [2];  [3];  [1];  [2];  [1]
  1. Univ. of Washington, Seattle, WA (United States)
  2. Univ. of California, San Diego, CA (United States)
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States); Swift Solar Inc., San Carlos, CA (United States)
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Adding a large A-site cation, such as dimethylammonium (DMA), to the perovskite growth solution has been shown to improve the performance and long-term operational stability of halide perovskite solar cells. To better understand the origins of these improvements, we explore the changes in film structure, composition, and optical properties of a formamidinium (FA), Cs, Pb, and mixed halide perovskite following the addition of DMA to the perovskite growth solution in the ratio of DMA0.1FA0.6Cs0.3Pb(I0.8Br0.2)3. Using time-of-flight secondary-ion mass spectrometry (TOF-SIMS), we show that DMA is indeed incorporated into the perovskite, with a higher DMA concentration at the surface. Using a combination of photoluminescence (PL) microscopy and photoinduced force microscopy-based (PiFM) nanoinfrared (nanoIR), we demonstrate that incorporating DMA into the film leads to increased local heterogeneity in the local bandgap and clustering of the local formamidinium (CH5N2+) composition. In addition, using nano-X-ray diffraction, we demonstrate that DMA incorporation also alters the local structural composition by changing the local d-spacing distribution and grain size. Our results suggest that compositional variations in the organic cations at the A-site drive the structural heterogeneity observed in the case of DMA-incorporated films. Our results also suggest that while current DMA-additive-based approaches do have benefits to operational stability and device performance, process optimization to achieve local compositional and structural homogeneity could further boost both of these gains in performance, bringing further gains to solar cells using DMA additives.

Research Organization:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Solar Energy Technologies Office; National Science Foundation (NSF)
Grant/Contract Number:
AC36-08GO28308; EE0008747
OSTI ID:
1841362
Alternate ID(s):
OSTI ID: 1844688
OSTI ID: 1845515
OSTI ID: 1910154
Report Number(s):
NREL/JA-5900-81917; MainId:82690; UUID:1e14934b-b953-40ad-ae79-79b62500e464; MainAdminID:63676
Journal Information:
ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 1 Vol. 7; ISSN 2380-8195
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (39)

Highly Efficient Perovskite-Perovskite Tandem Solar Cells Reaching 80% of the Theoretical Limit in Photovoltage journal July 2017
How To Quantify the Efficiency Potential of Neat Perovskite Films: Perovskite Semiconductors with an Implied Efficiency Exceeding 28% journal March 2020
Static time-of-flight secondary ion mass spectrometry and x-ray photoelectron spectroscopy characterization of adsorbed albumin and fibronectin films journal January 2001
Die Gesetze der Krystallochemie journal May 1926
Simplifying the interpretation of ToF-SIMS spectra and images using careful application of multivariate analysis journal July 2006
Detecting outliers: Do not use standard deviation around the mean, use absolute deviation around the median journal July 2013
Enabling Flexible All-Perovskite Tandem Solar Cells journal September 2019
Local Crystal Misorientation Influences Non-radiative Recombination in Halide Perovskites journal December 2019
Interpretation of Static Time-of-Flight Secondary Ion Mass Spectra of Adsorbed Protein Films by Multivariate Pattern Recognition journal March 2002
Linear and Nonlinear Optical Spectroscopy at the Nanoscale with Photoinduced Force Microscopy journal September 2015
Reducing Surface Recombination Velocity of Methylammonium-Free Mixed-Cation Mixed-Halide Perovskites via Surface Passivation journal June 2021
Identifying Nanoscale Structure–Function Relationships Using Multimodal Atomic Force Microscopy, Dimensionality Reduction, and Regression Techniques journal May 2018
Overcoming the Photovoltage Plateau in Large Bandgap Perovskite Photovoltaics journal May 2018
Probing Perovskite Inhomogeneity beyond the Surface: TOF-SIMS Analysis of Halide Perovskite Photovoltaic Devices journal July 2018
The Role of Dimethylammonium in Bandgap Modulation for Stable Halide Perovskites journal May 2020
Light-Induced Phase Segregation in Halide-Perovskite Absorbers journal November 2016
Defect-Assisted Photoinduced Halide Segregation in Mixed-Halide Perovskite Thin Films journal May 2017
Enhancing Defect Tolerance and Phase Stability of High-Bandgap Perovskites via Guanidinium Alloying journal May 2018
Reducing Surface Recombination Velocities at the Electrical Contacts Will Improve Perovskite Photovoltaics journal December 2018
Tracking Photoexcited Carriers in Hybrid Perovskite Semiconductors: Trap-Dominated Spatial Heterogeneity and Diffusion journal September 2017
A Reversible Structural Phase Transition by Electrochemically-Driven Ion Injection into a Conjugated Polymer journal March 2020
ToF-SIMS Analysis of Adsorbed Proteins: Principal Component Analysis of the Primary Ion Species Effect on the Protein Fragmentation Patterns journal November 2011
Photo-induced halide redistribution in organic–inorganic perovskite films journal May 2016
Hybrid perovskite films approaching the radiative limit with over 90% photoluminescence quantum efficiency journal April 2018
Metal halide perovskite tandem and multiple-junction photovoltaics journal November 2017
Reversible photo-induced trap formation in mixed-halide hybrid perovskites for photovoltaics journal January 2015
Cesium-containing triple cation perovskite solar cells: improved stability, reproducibility and high efficiency journal January 2016
Identifying and suppressing interfacial recombination to achieve high open-circuit voltage in perovskite solar cells journal January 2017
Insights into operational stability and processing of halide perovskite active layers journal January 2019
The impact of energy alignment and interfacial recombination on the internal and external open-circuit voltage of perovskite solar cells journal January 2019
Revealing the origin of voltage loss in mixed-halide perovskite solar cells journal January 2020
Enhanced mobility CsPbI 3 quantum dot arrays for record-efficiency, high-voltage photovoltaic cells journal October 2017
Impact of microstructure on local carrier lifetime in perovskite solar cells journal April 2015
A mixed-cation lead mixed-halide perovskite absorber for tandem solar cells journal January 2016
Homogenized halides and alkali cation segregation in alloyed organic-inorganic perovskites journal February 2019
Incorporation of rubidium cations into perovskite solar cells improves photovoltaic performance journal September 2016
Promises and challenges of perovskite solar cells journal November 2017
Triple-halide wide–band gap perovskites with suppressed phase segregation for efficient tandems journal March 2020
Analysis of variance, coefficient of determination and F-test for local polynomial regression journal October 2008

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Related Subjects

36 MATERIALS SCIENCE
additives
lead compounds
optical properties
optimization
perovskite solar cells
positive ions
secondary ion mass spectrometry