Local Background Hole Density Drives Nonradiative Recombination in Tin Halide Perovskites

Westbrook, Robert J. E.; Taddei, Margherita; Giridharagopal, Rajiv; Jiang, Meihuizi; Gallagher, Shaun M.; Guye, Kathryn N.; Warga, Aaron I.; Haque, Saif A.; Ginger, David S.

doi:10.1021/acsenergylett.3c02701

Local Background Hole Density Drives Nonradiative Recombination in Tin Halide Perovskites

Journal Article · Tue Jan 30 23:00:00 EST 2024 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.3c02701· OSTI ID:2395920

Westbrook, Robert J. E. ^[1]; ^[1]; ^[1]; Jiang, Meihuizi ^[2]; Gallagher, Shaun M. ^[1]; ^[1]; ^[1]; ^[2]; ^[3]

Univ. of Washington, Seattle, WA (United States)
Imperial College, London (United Kingdom)
Univ. of Washington, Seattle, WA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

In this study, we use multimodal microscopy to study carrier recombination in semiconducting tin halide perovskite films based on PEA_0.2FA_0.8SnI₃ (PEA = phenethylammonium; FA = formamidinium). We use the observation of pseudo-first-order photoluminescence (PL) decay kinetics to establish a method for quantifying the hole dopant level and nonradiative recombination rate constant. We find that untreated PEA_0.2FA_0.8SnI₃ films exhibit large hole doping concentrations of p₀ ≈ 10¹⁹ cm^–3, which is reduced to p₀ ≈ 10¹⁶ cm^–3 after SnF₂ treatment. While it is well-known that the radiative recombination rates are increased with p₀, we reveal that the nonradiative rate is also increased. We find that p-type regions in untreated PEA_0.2FA_0.8SnI₃ films are centers for nonradiative recombination, which are diminished in films with p₀ ≈ 10¹⁶ cm^–3. We discover significant PL heterogeneity even in PEA_0.2FA_0.8SnI₃ films with moderate dopant levels, suggesting that new strategies to eliminate deleterious defects in PEA_0.2FA_0.8SnI₃ must be developed.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Engineering and Physical Sciences Research Council (EPSRC)

Grant/Contract Number:: AC05-76RL01830; SC0013957

OSTI ID:: 2395920

Report Number(s):: PNNL-SA--190689

Journal Information:: ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 2 Vol. 9; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (47)

Cooling, Scattering, and Recombination—The Role of the Material Quality for the Physics of Tin Halide Perovskites Kahmann, Simon; Shao, Shuyan; Loi, Maria A. Advanced Functional Materials, Vol. 29, Issue 35 https://doi.org/10.1002/adfm.201902963	journal	June 2019
Lead-Free Inverted Planar Formamidinium Tin Triiodide Perovskite Solar Cells Achieving Power Conversion Efficiencies up to 6.22% Liao, Weiqiang; Zhao, Dewei; Yu, Yue Advanced Materials, Vol. 28, Issue 42 https://doi.org/10.1002/adma.201602992	journal	August 2016
The Effects of Doping Density and Temperature on the Optoelectronic Properties of Formamidinium Tin Triiodide Thin Films Milot, Rebecca L.; Klug, Matthew T.; Davies, Christopher L. Advanced Materials, Vol. 30, Issue 44 https://doi.org/10.1002/adma.201804506	journal	September 2018
Optoelectronic Properties of Low‐Bandgap Halide Perovskites for Solar Cell Applications Dey, Krishanu; Roose, Bart; Stranks, Samuel D. Advanced Materials, Vol. 33, Issue 40 https://doi.org/10.1002/adma.202102300	journal	August 2021
Tin Halide Perovskites: From Fundamental Properties to Solar Cells Pitaro, Matteo; Tekelenburg, Eelco Kinsa; Shao, Shuyan Advanced Materials, Vol. 34, Issue 1 https://doi.org/10.1002/adma.202105844	journal	October 2021
Engineering Stable Lead‐Free Tin Halide Perovskite Solar Cells: Lessons from Materials Chemistry Macdonald, Thomas J.; Lanzetta, Luis; Liang, Xinxing Advanced Materials, Vol. 35, Issue 25 https://doi.org/10.1002/adma.202206684	journal	April 2023
Highly Reproducible Sn-Based Hybrid Perovskite Solar Cells with 9% Efficiency Shao, Shuyan; Liu, Jian; Portale, Giuseppe Advanced Energy Materials, Vol. 8, Issue 4 https://doi.org/10.1002/aenm.201702019	journal	September 2017
Unveiling Roles of Tin Fluoride Additives in High‐Efficiency Low‐Bandgap Mixed Tin‐Lead Perovskite Solar Cells Chen, Qiyu; Luo, Jincheng; He, Rui Advanced Energy Materials, Vol. 11, Issue 29 https://doi.org/10.1002/aenm.202101045	journal	June 2021
Universal Current Losses in Perovskite Solar Cells Due to Mobile Ions Thiesbrummel, Jarla; Le Corre, Vincent M.; Peña‐Camargo, Francisco Advanced Energy Materials, Vol. 11, Issue 34 https://doi.org/10.1002/aenm.202101447	journal	July 2021
Engineering Perovskite Precursor Inks for Scalable Production of High‐Efficiency Perovskite Photovoltaic Modules Chung, Jaehoon; Kim, Seung‐Woo; Li, You Advanced Energy Materials, Vol. 13, Issue 22 https://doi.org/10.1002/aenm.202300595	journal	April 2023
Halide Chemistry in Tin Perovskite Optoelectronics: Bottlenecks and Opportunities Lanzetta, Luis; Webb, Thomas; Marin‐Beloqui, Jose Manuel Angewandte Chemie International Edition, Vol. 62, Issue 8 https://doi.org/10.1002/anie.202213966	journal	December 2022
Efficient and Stable FASnI ₃ Perovskite Solar Cells with Effective Interface Modulation by Low‐Dimensional Perovskite Layer Liao, Min; Yu, Bin‐Bin; Jin, Zhixin ChemSusChem, Vol. 12, Issue 22 https://doi.org/10.1002/cssc.201902000	journal	October 2019
Toward Understanding the Short‐Circuit Current Loss in Perovskite Solar Cells with 2D Passivation Layers Herterich, Jan; Baretzky, Clemens; Unmüssig, Moritz Solar RRL, Vol. 6, Issue 7 https://doi.org/10.1002/solr.202200195	journal	April 2022
Local Crystal Misorientation Influences Non-radiative Recombination in Halide Perovskites Jariwala, Sarthak; Sun, Hongyu; Adhyaksa, Gede W. P. Joule, Vol. 3, Issue 12 https://doi.org/10.1016/j.joule.2019.09.001	journal	December 2019
Tin perovskite solar cells with >1,300 h of operational stability in N2 through a synergistic chemical engineering approach Sanchez-Diaz, Jesús; Sánchez, Rafael S.; Masi, Sofia Joule, Vol. 6, Issue 4 https://doi.org/10.1016/j.joule.2022.02.014	journal	April 2022
Tin versus Lead Redox Chemistry Modulates Charge Trapping and Self-Doping in Tin/Lead Iodide Perovskites Meggiolaro, Daniele; Ricciarelli, Damiano; Alasmari, Ahmed A. The Journal of Physical Chemistry Letters, Vol. 11, Issue 9 https://doi.org/10.1021/acs.jpclett.0c00725	journal	April 2020
2D Phase Purity Determines Charge-Transfer Yield at 3D/2D Lead Halide Perovskite Heterojunctions Westbrook, Robert J. E.; Xu, Weidong; Liang, Xinxing The Journal of Physical Chemistry Letters, Vol. 12, Issue 13 https://doi.org/10.1021/acs.jpclett.1c00362	journal	March 2021
Surface Passivation Suppresses Local Ion Motion in Halide Perovskites Pothoof, Justin; Westbrook, Robert J. E.; Giridharagopal, Rajiv The Journal of Physical Chemistry Letters, Vol. 14, Issue 26 https://doi.org/10.1021/acs.jpclett.3c01089	journal	June 2023
Instability of Tin Iodide Perovskites: Bulk p-Doping versus Surface Tin Oxidation Ricciarelli, Damiano; Meggiolaro, Daniele; Ambrosio, Francesco ACS Energy Letters, Vol. 5, Issue 9 https://doi.org/10.1021/acsenergylett.0c01174	journal	July 2020
Optoelectronic Properties of Tin–Lead Halide Perovskites Savill, Kimberley J.; Ulatowski, Aleksander M.; Herz, Laura M. ACS Energy Letters, Vol. 6, Issue 7 https://doi.org/10.1021/acsenergylett.1c00776	journal	June 2021
Dimethylammonium Addition to Halide Perovskite Precursor Increases Vertical and Lateral Heterogeneity Jariwala, Sarthak; Kumar, Rishi E.; Eperon, Giles E. ACS Energy Letters, Vol. 7, Issue 1 https://doi.org/10.1021/acsenergylett.1c02302	journal	December 2021
(3-Aminopropyl)trimethoxysilane Surface Passivation Improves Perovskite Solar Cell Performance by Reducing Surface Recombination Velocity Shi, Yangwei; Rojas-Gatjens, Esteban; Wang, Jian ACS Energy Letters, Vol. 7, Issue 11 https://doi.org/10.1021/acsenergylett.2c01766	journal	October 2022
Ethylenediamine Addition Improves Performance and Suppresses Phase Instabilities in Mixed-Halide Perovskites Taddei, Margherita; Smith, Joel A.; Gallant, Benjamin M. ACS Energy Letters, Vol. 7, Issue 12 https://doi.org/10.1021/acsenergylett.2c01998	journal	November 2022
Photoluminescence Lifetimes Exceeding 8 μs and Quantum Yields Exceeding 30% in Hybrid Perovskite Thin Films by Ligand Passivation deQuilettes, Dane W.; Koch, Susanne; Burke, Sven ACS Energy Letters, Vol. 1, Issue 2 https://doi.org/10.1021/acsenergylett.6b00236	journal	July 2016
Reducing Carrier Density in Formamidinium Tin Perovskites and Its Beneficial Effects on Stability and Efficiency of Perovskite Solar Cells Lee, Seon Joo; Shin, Seong Sik; Im, Jino ACS Energy Letters, Vol. 3, Issue 1 https://doi.org/10.1021/acsenergylett.7b00976	journal	November 2017
Reducing Surface Recombination Velocities at the Electrical Contacts Will Improve Perovskite Photovoltaics Wang, Jian; Fu, Weifei; Jariwala, Sarthak ACS Energy Letters, Vol. 4, Issue 1 https://doi.org/10.1021/acsenergylett.8b02058	journal	December 2018
One-Step Synthesis of SnI ₂ ·(DMSO) _x Adducts for High-Performance Tin Perovskite Solar Cells Jiang, Xianyuan; Li, Hansheng; Zhou, Qilin Journal of the American Chemical Society, Vol. 143, Issue 29 https://doi.org/10.1021/jacs.1c03032	journal	July 2021
Lewis Base Passivation Mediates Charge Transfer at Perovskite Heterojunctions Westbrook, Robert J. E.; Macdonald, Thomas J.; Xu, Weidong Journal of the American Chemical Society, Vol. 143, Issue 31 https://doi.org/10.1021/jacs.1c05122	journal	August 2021
Fabrication of Efficient Formamidinium Tin Iodide Perovskite Solar Cells through SnF ₂ –Pyrazine Complex Lee, Seon Joo; Shin, Seong Sik; Kim, Young Chan Journal of the American Chemical Society, Vol. 138, Issue 12 https://doi.org/10.1021/jacs.6b00142	journal	March 2016
Spectral Control of Plasmonic Emission Enhancement from Quantum Dots near Single Silver Nanoprisms Munechika, Keiko; Chen, Yeechi; Tillack, Andreas F. Nano Letters, Vol. 10, Issue 7 https://doi.org/10.1021/nl101281a	journal	May 2010
Sn(IV)-free tin perovskite films realized by in situ Sn(0) nanoparticle treatment of the precursor solution Nakamura, Tomoya; Yakumaru, Shinya; Truong, Minh Anh Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-16726-3	journal	June 2020
Degradation mechanism of hybrid tin-based perovskite solar cells and the critical role of tin (IV) iodide Lanzetta, Luis; Webb, Thomas; Zibouche, Nourdine Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-22864-z	journal	May 2021
High-performance hysteresis-free perovskite transistors through anion engineering Zhu, Huihui; Liu, Ao; Shim, Kyu In Nature Communications, Vol. 13, Issue 1 https://doi.org/10.1038/s41467-022-29434-x	journal	April 2022
Monolithic all-perovskite tandem solar cells with 24.8% efficiency exploiting comproportionation to suppress Sn(ii) oxidation in precursor ink Lin, Renxing; Xiao, Ke; Qin, Zhengyuan Nature Energy, Vol. 4, Issue 10 https://doi.org/10.1038/s41560-019-0466-3	journal	September 2019
Nanoscale chemical heterogeneity dominates the optoelectronic response of alloyed perovskite solar cells Frohna, Kyle; Anaya, Miguel; Macpherson, Stuart Nature Nanotechnology, Vol. 17, Issue 2 https://doi.org/10.1038/s41565-021-01019-7	journal	November 2021
Photodoping through local charge carrier accumulation in alloyed hybrid perovskites for highly efficient luminescence Feldmann, Sascha; Macpherson, Stuart; Senanayak, Satyaprasad P. Nature Photonics, Vol. 14, Issue 2 https://doi.org/10.1038/s41566-019-0546-8	journal	November 2019
Performance-limiting nanoscale trap clusters at grain junctions in halide perovskites Doherty, Tiarnan A. S.; Winchester, Andrew J.; Macpherson, Stuart Nature, Vol. 580, Issue 7803 https://doi.org/10.1038/s41586-020-2184-1	journal	April 2020
All-perovskite tandem solar cells with improved grain surface passivation Lin, Renxing; Xu, Jian; Wei, Mingyang Nature, Vol. 603, Issue 7899 https://doi.org/10.1038/s41586-021-04372-8	journal	January 2022
Origin of Sn( ii ) oxidation in tin halide perovskites Pascual, Jorge; Nasti, Giuseppe; Aldamasy, Mahmoud H. Materials Advances, Vol. 1, Issue 5 https://doi.org/10.1039/D0MA00245C	journal	January 2020
Effect of electronic doping and traps on carrier dynamics in tin halide perovskites Treglia, Antonella; Ambrosio, Francesco; Martani, Samuele Materials Horizons, Vol. 9, Issue 6 https://doi.org/10.1039/D2MH00008C	journal	January 2022
Enhancing the performance of tin-based perovskite solar cells through solvent purification of tin iodide Zeng, Guojun; Pu, Dexin; Huang, Lishuai Journal of Materials Chemistry A, Vol. 11, Issue 21 https://doi.org/10.1039/D3TA01197F	journal	January 2023
Band‐gap narrowing in novel III‐V semiconductors Jain, S. C.; McGregor, J. M.; Roulston, D. J. Journal of Applied Physics, Vol. 68, Issue 7 https://doi.org/10.1063/1.346291	journal	October 1990
Impact of microstructure on local carrier lifetime in perovskite solar cells de Quilettes, D. W.; Vorpahl, S. M.; Stranks, S. D. Science, Vol. 348, Issue 6235 https://doi.org/10.1126/science.aaa5333	journal	April 2015
Perovskite-perovskite tandem photovoltaics with optimized band gaps Eperon, Giles E.; Leijtens, Tomas; Bush, Kevin A. Science, Vol. 354, Issue 6314 https://doi.org/10.1126/science.aaf9717	journal	October 2016
Homogenized halides and alkali cation segregation in alloyed organic-inorganic perovskites Correa-Baena, Juan-Pablo; Luo, Yanqi; Brenner, Thomas M. Science, Vol. 363, Issue 6427 https://doi.org/10.1126/science.aah5065	journal	February 2019
Resolving spatial and energetic distributions of trap states in metal halide perovskite solar cells Ni, Zhenyi; Bao, Chunxiong; Liu, Ye Science, Vol. 367, Issue 6484 https://doi.org/10.1126/science.aba0893	journal	March 2020
The Physics of Solar Cells Nelson, Jenny World Scientific https://doi.org/10.1142/p276	book	January 2003

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