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Title: A quantitative and spatially resolved analysis of the performance-bottleneck in high efficiency, planar hybrid perovskite solar cells

Abstract

Hybrid perovskites represent a potential paradigm shift for the creation of low-cost solar cells. Current power conversion efficiencies (PCEs) exceed 22%. However, despite this, record PCEs are still far from their theoretical Shockley–Queisser limit of 31%. To increase these PCE values, there is a pressing need to understand, quantify and microscopically model charge recombination processes in full working devices. Here, we present a complete microscopic account of charge recombination processes in high efficiency (18–19% PCE) hybrid perovskite (mixed cation and methylammonium lead iodide) solar cells. We employ diffraction-limited optical measurements along with relevant kinetic modeling to establish, for the first time, local photoluminescence quantum yields, trap densities, trapping efficiencies, charge extraction efficiencies, quasi-Fermi-level splitting, and effective PCE estimates. Correlations between these spatially resolved parameters, in turn, allow us to conclude that intrinsic electron traps in the perovskite active layers limit the performance of these state-of-the-art hybrid perovskite solar cells.

Authors:
 [1]; ORCiD logo [2];  [3];  [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [3]
  1. Univ. of Notre Dame, IN (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  3. Univ. of Notre Dame, IN (United States). Notre Dame Radiation Lab. (NDRL)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1429608
Report Number(s):
NREL/JA-5900-70074
Journal ID: ISSN 1754-5692
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Energy & Environmental Science
Additional Journal Information:
Journal Volume: 11; Journal Issue: 4; Journal ID: ISSN 1754-5692
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE; perovskite solar cells; power conversion efficiency; recombination

Citation Formats

Draguta, Sergiu, Christians, Jeffrey A., Morozov, Yurii V., Mucunzi, Anselme, Manser, Joseph S., Kamat, Prashant V., Luther, Joseph M., and Kuno, Masaru. A quantitative and spatially resolved analysis of the performance-bottleneck in high efficiency, planar hybrid perovskite solar cells. United States: N. p., 2018. Web. doi:10.1039/C7EE03654J.
Draguta, Sergiu, Christians, Jeffrey A., Morozov, Yurii V., Mucunzi, Anselme, Manser, Joseph S., Kamat, Prashant V., Luther, Joseph M., & Kuno, Masaru. A quantitative and spatially resolved analysis of the performance-bottleneck in high efficiency, planar hybrid perovskite solar cells. United States. doi:10.1039/C7EE03654J.
Draguta, Sergiu, Christians, Jeffrey A., Morozov, Yurii V., Mucunzi, Anselme, Manser, Joseph S., Kamat, Prashant V., Luther, Joseph M., and Kuno, Masaru. Mon . "A quantitative and spatially resolved analysis of the performance-bottleneck in high efficiency, planar hybrid perovskite solar cells". United States. doi:10.1039/C7EE03654J. https://www.osti.gov/servlets/purl/1429608.
@article{osti_1429608,
title = {A quantitative and spatially resolved analysis of the performance-bottleneck in high efficiency, planar hybrid perovskite solar cells},
author = {Draguta, Sergiu and Christians, Jeffrey A. and Morozov, Yurii V. and Mucunzi, Anselme and Manser, Joseph S. and Kamat, Prashant V. and Luther, Joseph M. and Kuno, Masaru},
abstractNote = {Hybrid perovskites represent a potential paradigm shift for the creation of low-cost solar cells. Current power conversion efficiencies (PCEs) exceed 22%. However, despite this, record PCEs are still far from their theoretical Shockley–Queisser limit of 31%. To increase these PCE values, there is a pressing need to understand, quantify and microscopically model charge recombination processes in full working devices. Here, we present a complete microscopic account of charge recombination processes in high efficiency (18–19% PCE) hybrid perovskite (mixed cation and methylammonium lead iodide) solar cells. We employ diffraction-limited optical measurements along with relevant kinetic modeling to establish, for the first time, local photoluminescence quantum yields, trap densities, trapping efficiencies, charge extraction efficiencies, quasi-Fermi-level splitting, and effective PCE estimates. Correlations between these spatially resolved parameters, in turn, allow us to conclude that intrinsic electron traps in the perovskite active layers limit the performance of these state-of-the-art hybrid perovskite solar cells.},
doi = {10.1039/C7EE03654J},
journal = {Energy & Environmental Science},
number = 4,
volume = 11,
place = {United States},
year = {2018},
month = {2}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Figures / Tables:

Fig. 1 Fig. 1: Fig. 1a first shows a schematic of the FAMACs and MAPbI3 solar cells being studied with device cross-sectional scanning electron micrographs (SEMs) shown in Fig. 1b. In each case, the perovskite layer thickness is ~500 nm with 2,2',7,7'-tetrakis(N,N-di-pmethox phen lamino)-9,9'-spirobifluorene (Spiro-OMeTAD) as the HTL and TiO2 as themore » ETL. Champion (average) PCEs are 18.9% (17.9%) and 17.8% (16.5%), respectively (Fig. 1c, see ESI (Electronic Supplementary Information)« less

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Works referenced in this record:

Intriguing Optoelectronic Properties of Metal Halide Perovskites
journal, June 2016


High-Work-Function Molybdenum Oxide Hole Extraction Contacts in Hybrid Organic–Inorganic Perovskite Solar Cells
journal, November 2016

  • Schulz, Philip; Tiepelt, Jan O.; Christians, Jeffrey A.
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 46
  • DOI: 10.1021/acsami.6b10898

Spatial Localization of Excitons and Charge Carriers in Hybrid Perovskite Thin Films
journal, July 2015

  • Simpson, Mary Jane; Doughty, Benjamin; Yang, Bin
  • The Journal of Physical Chemistry Letters, Vol. 6, Issue 15
  • DOI: 10.1021/acs.jpclett.5b01050

Band filling with free charge carriers in organometal halide perovskites
journal, August 2014


Anticorrelation between Local Photoluminescence and Photocurrent Suggests Variability in Contact to Active Layer in Perovskite Solar Cells
journal, October 2016


Charge-Carrier Mobilities in Metal Halide Perovskites: Fundamental Mechanisms and Limits
journal, June 2017


Temperature-Dependent Charge-Carrier Dynamics in CH 3 NH 3 PbI 3 Perovskite Thin Films
journal, September 2015

  • Milot, Rebecca L.; Eperon, Giles E.; Snaith, Henry J.
  • Advanced Functional Materials, Vol. 25, Issue 39
  • DOI: 10.1002/adfm.201502340

Top and bottom surfaces limit carrier lifetime in lead iodide perovskite films
journal, January 2017


High Photoluminescence Quantum Yield in Band Gap Tunable Bromide Containing Mixed Halide Perovskites
journal, December 2015


Impedance Spectroscopic Analysis of Lead Iodide Perovskite-Sensitized Solid-State Solar Cells
journal, December 2013

  • Dualeh, Amalie; Moehl, Thomas; Tétreault, Nicolas
  • ACS Nano, Vol. 8, Issue 1, p. 362-373
  • DOI: 10.1021/nn404323g

Charge Injection at the Heterointerface in Perovskite CH 3 NH 3 PbI 3 Solar Cells Studied by Simultaneous Microscopic Photoluminescence and Photocurrent Imaging Spectroscopy
journal, August 2016

  • Yamashita, Daiki; Handa, Taketo; Ihara, Toshiyuki
  • The Journal of Physical Chemistry Letters, Vol. 7, Issue 16
  • DOI: 10.1021/acs.jpclett.6b01231

Unravelling the mechanism of photoinduced charge transfer processes in lead iodide perovskite solar cells
journal, January 2014

  • Marchioro, Arianna; Teuscher, Joël; Friedrich, Dennis
  • Nature Photonics, Vol. 8, Issue 3
  • DOI: 10.1038/nphoton.2013.374

Highly Reproducible Perovskite Solar Cells with Average Efficiency of 18.3% and Best Efficiency of 19.7% Fabricated via Lewis Base Adduct of Lead(II) Iodide
journal, July 2015

  • Ahn, Namyoung; Son, Dae-Yong; Jang, In-Hyuk
  • Journal of the American Chemical Society, Vol. 137, Issue 27
  • DOI: 10.1021/jacs.5b04930

Carrier separation and transport in perovskite solar cells studied by nanometre-scale profiling of electrical potential
journal, September 2015

  • Jiang, Chun-Sheng; Yang, Mengjin; Zhou, Yuanyuan
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9397

Device modeling of perovskite solar cells based on structural similarity with thin film inorganic semiconductor solar cells
journal, August 2014

  • Minemoto, Takashi; Murata, Masashi
  • Journal of Applied Physics, Vol. 116, Issue 5
  • DOI: 10.1063/1.4891982

Strong Covalency-Induced Recombination Centers in Perovskite Solar Cell Material CH 3 NH 3 PbI 3
journal, October 2014

  • Agiorgousis, Michael L.; Sun, Yi-Yang; Zeng, Hao
  • Journal of the American Chemical Society, Vol. 136, Issue 41
  • DOI: 10.1021/ja5079305

Recombination Kinetics in Organic-Inorganic Perovskites: Excitons, Free Charge, and Subgap States
journal, September 2014


Characterization of Planar Lead Halide Perovskite Solar Cells by Impedance Spectroscopy, Open-Circuit Photovoltage Decay, and Intensity-Modulated Photovoltage/Photocurrent Spectroscopy
journal, February 2015

  • Pockett, Adam; Eperon, Giles E.; Peltola, Timo
  • The Journal of Physical Chemistry C, Vol. 119, Issue 7
  • DOI: 10.1021/jp510837q

The Controlling Mechanism for Potential Loss in CH 3 NH 3 PbBr 3 Hybrid Solar Cells
journal, July 2016


Correlating Photoluminescence Heterogeneity with Local Electronic Properties in Methylammonium Lead Tribromide Perovskite Thin Films
journal, June 2017


Quantifying Efficiency Loss of Perovskite Solar Cells by a Modified Detailed Balance Model
journal, December 2017

  • Sha, Wei E. I.; Zhang, Hong; Wang, Zi Shuai
  • Advanced Energy Materials, Vol. 8, Issue 8
  • DOI: 10.1002/aenm.201701586

Efficient and Balanced Charge Transport Revealed in Planar Perovskite Solar Cells
journal, February 2015

  • Chen, Yani; Peng, Jiajun; Su, Diqing
  • ACS Applied Materials & Interfaces, Vol. 7, Issue 8
  • DOI: 10.1021/acsami.5b00077

Spatial and temporal imaging of long-range charge transport in perovskite thin films by ultrafast microscopy
journal, June 2015

  • Guo, Zhi; Manser, Joseph S.; Wan, Yan
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8471

Interface energetics in organo-metal halide perovskite-based photovoltaic cells
journal, January 2014

  • Schulz, Philip; Edri, Eran; Kirmayer, Saar
  • Energy & Environmental Science, Vol. 7, Issue 4
  • DOI: 10.1039/c4ee00168k

High Photoluminescence Efficiency and Optically Pumped Lasing in Solution-Processed Mixed Halide Perovskite Semiconductors
journal, March 2014

  • Deschler, Felix; Price, Michael; Pathak, Sandeep
  • The Journal of Physical Chemistry Letters, Vol. 5, Issue 8
  • DOI: 10.1021/jz5005285

Efficient charge extraction and slow recombination in organic–inorganic perovskites capped with semiconducting single-walled carbon nanotubes
journal, January 2016

  • Ihly, Rachelle; Dowgiallo, Anne-Marie; Yang, Mengjin
  • Energy & Environmental Science, Vol. 9, Issue 4
  • DOI: 10.1039/C5EE03806E

Trap States in Lead Iodide Perovskites
journal, January 2015

  • Wu, Xiaoxi; Trinh, M. Tuan; Niesner, Daniel
  • Journal of the American Chemical Society, Vol. 137, Issue 5
  • DOI: 10.1021/ja512833n

Monitoring a Silent Phase Transition in CH 3 NH 3 PbI 3 Solar Cells via Operando X-ray Diffraction
journal, October 2016


Analysis of Photoinduced Carrier Recombination Kinetics in Flat and Mesoporous Lead Perovskite Solar Cells
journal, December 2016


Impact of microstructure on local carrier lifetime in perovskite solar cells
journal, April 2015


Correlated electron–hole plasma in organometal perovskites
journal, September 2014

  • Saba, Michele; Cadelano, Michele; Marongiu, Daniela
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms6049

The efficiency limit of CH 3 NH 3 PbI 3 perovskite solar cells
journal, June 2015

  • Sha, Wei E. I.; Ren, Xingang; Chen, Luzhou
  • Applied Physics Letters, Vol. 106, Issue 22
  • DOI: 10.1063/1.4922150

Carrier recombination dynamics in individual CdSe nanowires
journal, March 2011


Cesium-containing triple cation perovskite solar cells: improved stability, reproducibility and high efficiency
journal, January 2016

  • Saliba, Michael; Matsui, Taisuke; Seo, Ji-Youn
  • Energy & Environmental Science, Vol. 9, Issue 6
  • DOI: 10.1039/C5EE03874J

Carrier trapping and recombination: the role of defect physics in enhancing the open circuit voltage of metal halide perovskite solar cells
journal, January 2016

  • Leijtens, Tomas; Eperon, Giles E.; Barker, Alex J.
  • Energy & Environmental Science, Vol. 9, Issue 11
  • DOI: 10.1039/C6EE01729K

Multifaceted Excited State of CH 3 NH 3 PbI 3 . Charge Separation, Recombination, and Trapping
journal, May 2015

  • Christians, Jeffrey A.; Manser, Joseph S.; Kamat, Prashant V.
  • The Journal of Physical Chemistry Letters, Vol. 6, Issue 11
  • DOI: 10.1021/acs.jpclett.5b00594

Numerical simulation: Toward the design of high-efficiency planar perovskite solar cells
journal, June 2014

  • Liu, Feng; Zhu, Jun; Wei, Junfeng
  • Applied Physics Letters, Vol. 104, Issue 25
  • DOI: 10.1063/1.4885367

Facet-dependent photovoltaic efficiency variations in single grains of hybrid halide perovskite
journal, July 2016


Micrometer Sized Perovskite Crystals in Planar Hole Conductor Free Solar Cells
journal, August 2015

  • Gamliel, Shany; Dymshits, Alex; Aharon, Sigalit
  • The Journal of Physical Chemistry C, Vol. 119, Issue 34
  • DOI: 10.1021/acs.jpcc.5b07554

Comparison of Recombination Dynamics in CH 3 NH 3 PbBr 3 and CH 3 NH 3 PbI 3 Perovskite Films: Influence of Exciton Binding Energy
journal, November 2015


Incorporation of rubidium cations into perovskite solar cells improves photovoltaic performance
journal, September 2016


Detailed Balance Limit of Efficiency of p‐n Junction Solar Cells
journal, March 1961

  • Shockley, William; Queisser, Hans J.
  • Journal of Applied Physics, Vol. 32, Issue 3, p. 510-519
  • DOI: 10.1063/1.1736034

Optoelectronic Quality and Stability of Hybrid Perovskites from MAPbI 3 to MAPbI 2 Br Using Composition Spread Libraries
journal, January 2016

  • Braly, Ian L.; Hillhouse, Hugh W.
  • The Journal of Physical Chemistry C, Vol. 120, Issue 2
  • DOI: 10.1021/acs.jpcc.5b10728

Structural and optical properties of methylammonium lead iodide across the tetragonal to cubic phase transition: implications for perovskite solar cells
journal, January 2016

  • Quarti, Claudio; Mosconi, Edoardo; Ball, James M.
  • Energy & Environmental Science, Vol. 9, Issue 1
  • DOI: 10.1039/C5EE02925B

Photoluminescence Lifetimes Exceeding 8 μs and Quantum Yields Exceeding 30% in Hybrid Perovskite Thin Films by Ligand Passivation
journal, July 2016


Improved Carrier Transport in Perovskite Solar Cells Probed by Femtosecond Transient Absorption Spectroscopy
journal, December 2017

  • Serpetzoglou, Efthymis; Konidakis, Ioannis; Kakavelakis, George
  • ACS Applied Materials & Interfaces, Vol. 9, Issue 50
  • DOI: 10.1021/acsami.7b15195

Mapping the Photoresponse of CH 3 NH 3 PbI 3 Hybrid Perovskite Thin Films at the Nanoscale
journal, May 2016


Spatially Non-uniform Trap State Densities in Solution-Processed Hybrid Perovskite Thin Films
journal, February 2016

  • Draguta, Sergiu; Thakur, Siddharatha; Morozov, Yurii V.
  • The Journal of Physical Chemistry Letters, Vol. 7, Issue 4
  • DOI: 10.1021/acs.jpclett.5b02888

Efficient carrier transport in halide perovskites: theoretical perspectives
journal, January 2014


Exploring the Way To Approach the Efficiency Limit of Perovskite Solar Cells by Drift-Diffusion Model
journal, March 2017


Observation of a hot-phonon bottleneck in lead-iodide perovskites
journal, October 2015


    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.