DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Triple-halide wide–band gap perovskites with suppressed phase segregation for efficient tandems

Abstract

Wide–band gap metal halide perovskites are promising semiconductors to pair with silicon in tandem solar cells to pursue the goal of achieving power conversion efficiency (PCE) greater than 30% at low cost. However, wide–band gap perovskite solar cells have been fundamentally limited by photoinduced phase segregation and low open-circuit voltage. We report efficient 1.67–electron volt wide–band gap perovskite top cells using triple-halide alloys (chlorine, bromine, iodine) to tailor the band gap and stabilize the semiconductor under illumination. We show a factor of 2 increase in photocarrier lifetime and charge-carrier mobility that resulted from enhancing the solubility of chlorine by replacing some of the iodine with bromine to shrink the lattice parameter. We observed a suppression of light-induced phase segregation in films even at 100-sun illumination intensity and less than 4% degradation in semitransparent top cells after 1000 hours of maximum power point (MPP) operation at 60°C. By integrating these top cells with silicon bottom cells, we achieved a PCE of 27% in two-terminal monolithic tandems with an area of 1 square centimeter.

Authors:
ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ; ORCiD logo; ORCiD logo; ORCiD logo; ; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States); Stanford Univ., CA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office; National Science Foundation (NSF); US Department of the Navy, Office of Naval Research (ONR)
OSTI Identifier:
1603222
Alternate Identifier(s):
OSTI ID: 1605080; OSTI ID: 1686148
Report Number(s):
NREL/JA-5900-75003
Journal ID: ISSN 0036-8075; /sci/367/6482/1097.atom
Grant/Contract Number:  
EE0008167; AC36-08GO23808; AC36-08GO28308; DGE-1656518; N00014-17-1-2525
Resource Type:
Published Article
Journal Name:
Science
Additional Journal Information:
Journal Name: Science Journal Volume: 367 Journal Issue: 6482; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE; Halide perovskites; semiconductors; tandem solar cells; power conversion efficiency

Citation Formats

Xu, Jixian, Boyd, Caleb C., Yu, Zhengshan J., Palmstrom, Axel F., Witter, Daniel J., Larson, Bryon W., France, Ryan M., Werner, Jérémie, Harvey, Steven P., Wolf, Eli J., Weigand, William, Manzoor, Salman, van Hest, Maikel F. A. M., Berry, Joseph J., Luther, Joseph M., Holman, Zachary C., and McGehee, Michael D. Triple-halide wide–band gap perovskites with suppressed phase segregation for efficient tandems. United States: N. p., 2020. Web. doi:10.1126/science.aaz5074.
Xu, Jixian, Boyd, Caleb C., Yu, Zhengshan J., Palmstrom, Axel F., Witter, Daniel J., Larson, Bryon W., France, Ryan M., Werner, Jérémie, Harvey, Steven P., Wolf, Eli J., Weigand, William, Manzoor, Salman, van Hest, Maikel F. A. M., Berry, Joseph J., Luther, Joseph M., Holman, Zachary C., & McGehee, Michael D. Triple-halide wide–band gap perovskites with suppressed phase segregation for efficient tandems. United States. https://doi.org/10.1126/science.aaz5074
Xu, Jixian, Boyd, Caleb C., Yu, Zhengshan J., Palmstrom, Axel F., Witter, Daniel J., Larson, Bryon W., France, Ryan M., Werner, Jérémie, Harvey, Steven P., Wolf, Eli J., Weigand, William, Manzoor, Salman, van Hest, Maikel F. A. M., Berry, Joseph J., Luther, Joseph M., Holman, Zachary C., and McGehee, Michael D. Fri . "Triple-halide wide–band gap perovskites with suppressed phase segregation for efficient tandems". United States. https://doi.org/10.1126/science.aaz5074.
@article{osti_1603222,
title = {Triple-halide wide–band gap perovskites with suppressed phase segregation for efficient tandems},
author = {Xu, Jixian and Boyd, Caleb C. and Yu, Zhengshan J. and Palmstrom, Axel F. and Witter, Daniel J. and Larson, Bryon W. and France, Ryan M. and Werner, Jérémie and Harvey, Steven P. and Wolf, Eli J. and Weigand, William and Manzoor, Salman and van Hest, Maikel F. A. M. and Berry, Joseph J. and Luther, Joseph M. and Holman, Zachary C. and McGehee, Michael D.},
abstractNote = {Wide–band gap metal halide perovskites are promising semiconductors to pair with silicon in tandem solar cells to pursue the goal of achieving power conversion efficiency (PCE) greater than 30% at low cost. However, wide–band gap perovskite solar cells have been fundamentally limited by photoinduced phase segregation and low open-circuit voltage. We report efficient 1.67–electron volt wide–band gap perovskite top cells using triple-halide alloys (chlorine, bromine, iodine) to tailor the band gap and stabilize the semiconductor under illumination. We show a factor of 2 increase in photocarrier lifetime and charge-carrier mobility that resulted from enhancing the solubility of chlorine by replacing some of the iodine with bromine to shrink the lattice parameter. We observed a suppression of light-induced phase segregation in films even at 100-sun illumination intensity and less than 4% degradation in semitransparent top cells after 1000 hours of maximum power point (MPP) operation at 60°C. By integrating these top cells with silicon bottom cells, we achieved a PCE of 27% in two-terminal monolithic tandems with an area of 1 square centimeter.},
doi = {10.1126/science.aaz5074},
journal = {Science},
number = 6482,
volume = 367,
place = {United States},
year = {Fri Mar 06 00:00:00 EST 2020},
month = {Fri Mar 06 00:00:00 EST 2020}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1126/science.aaz5074

Citation Metrics:
Cited by: 455 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Chemical Management for Colorful, Efficient, and Stable Inorganic–Organic Hybrid Nanostructured Solar Cells
journal, March 2013

  • Noh, Jun Hong; Im, Sang Hyuk; Heo, Jin Hyuck
  • Nano Letters, Vol. 13, Issue 4, p. 1764-1769
  • DOI: 10.1021/nl400349b

Vacuum-Deposited Blue Inorganic Perovskite Light-Emitting Diodes
journal, November 2019

  • Du, Peipei; Li, Jinghui; Wang, Liang
  • ACS Applied Materials & Interfaces, Vol. 11, Issue 50
  • DOI: 10.1021/acsami.9b17164

Stabilizing Perovskite Structures by Tuning Tolerance Factor: Formation of Formamidinium and Cesium Lead Iodide Solid-State Alloys
journal, December 2015


Generalized Optoelectronic Model of Series-Connected Multijunction Solar Cells
journal, November 2015


Balancing electrical and optical losses for efficient 4-terminal Si–perovskite solar cells with solution processed percolation electrodes
journal, January 2018

  • Ramírez Quiroz, César Omar; Shen, Yilei; Salvador, Michael
  • Journal of Materials Chemistry A, Vol. 6, Issue 8
  • DOI: 10.1039/C7TA10945H

High-Performance Planar-Heterojunction Solar Cells Based on Ternary Halide Large-Band-Gap Perovskites
journal, August 2014

  • Liang, Po-Wei; Chueh, Chu-Chen; Xin, Xu-Kai
  • Advanced Energy Materials, Vol. 5, Issue 1
  • DOI: 10.1002/aenm.201400960

Translation of device performance measurements to reference conditions
journal, September 1986


Opportunities and challenges for tandem solar cells using metal halide perovskite semiconductors
journal, July 2018


23.6%-efficient monolithic perovskite/silicon tandem solar cells with improved stability
journal, February 2017

  • Bush, Kevin A.; Palmstrom, Axel F.; Yu, Zhengshan J.
  • Nature Energy, Vol. 2, Issue 4
  • DOI: 10.1038/nenergy.2017.9

Interfacial Effects of Tin Oxide Atomic Layer Deposition in Metal Halide Perovskite Photovoltaics
journal, June 2018

  • Palmstrom, Axel F.; Raiford, James A.; Prasanna, Rohit
  • Advanced Energy Materials, Vol. 8, Issue 23
  • DOI: 10.1002/aenm.201800591

Reversible photo-induced trap formation in mixed-halide hybrid perovskites for photovoltaics
journal, January 2015

  • Hoke, Eric T.; Slotcavage, Daniel J.; Dohner, Emma R.
  • Chemical Science, Vol. 6, Issue 1
  • DOI: 10.1039/C4SC03141E

CH 3 NH 3 Sn x Pb (1– x ) I 3 Perovskite Solar Cells Covering up to 1060 nm
journal, March 2014

  • Ogomi, Yuhei; Morita, Atsushi; Tsukamoto, Syota
  • The Journal of Physical Chemistry Letters, Vol. 5, Issue 6
  • DOI: 10.1021/jz5002117

Shift Happens . How Halide Ion Defects Influence Photoinduced Segregation in Mixed Halide Perovskites
journal, June 2017


Efficient, stable solar cells by using inherent bandgap of α-phase formamidinium lead iodide
journal, November 2019


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


Homogenized halides and alkali cation segregation in alloyed organic-inorganic perovskites
journal, February 2019

  • Correa-Baena, Juan-Pablo; Luo, Yanqi; Brenner, Thomas M.
  • Science, Vol. 363, Issue 6427
  • DOI: 10.1126/science.aah5065

Rubidium Multication Perovskite with Optimized Bandgap for Perovskite-Silicon Tandem with over 26% Efficiency
journal, April 2017

  • Duong, The; Wu, YiLiang; Shen, Heping
  • Advanced Energy Materials, Vol. 7, Issue 14
  • DOI: 10.1002/aenm.201700228

Maximizing and stabilizing luminescence from halide perovskites with potassium passivation
journal, March 2018

  • Abdi-Jalebi, Mojtaba; Andaji-Garmaroudi, Zahra; Cacovich, Stefania
  • Nature, Vol. 555, Issue 7697
  • DOI: 10.1038/nature25989

Photovoltaic mixed-cation lead mixed-halide perovskites: links between crystallinity, photo-stability and electronic properties
journal, January 2017

  • Rehman, Waqaas; McMeekin, David P.; Patel, Jay B.
  • Energy & Environmental Science, Vol. 10, Issue 1
  • DOI: 10.1039/C6EE03014A

Techno-economic viability of silicon-based tandem photovoltaic modules in the United States
journal, July 2018


Formamidinium lead trihalide: a broadly tunable perovskite for efficient planar heterojunction solar cells
journal, January 2014

  • Eperon, Giles E.; Stranks, Samuel D.; Menelaou, Christopher
  • Energy & Environmental Science, Vol. 7, Issue 3
  • DOI: 10.1039/c3ee43822h

Cost Analysis of Perovskite Tandem Photovoltaics
journal, August 2018


Structural, optical, and electronic studies of wide-bandgap lead halide perovskites
journal, January 2015

  • Comin, Riccardo; Walters, Grant; Thibau, Emmanuel Sol
  • Journal of Materials Chemistry C, Vol. 3, Issue 34
  • DOI: 10.1039/C5TC01718A

Predicting and optimising the energy yield of perovskite-on-silicon tandem solar cells under real world conditions
journal, January 2017

  • Hörantner, Maximilian T.; Snaith, Henry J.
  • Energy & Environmental Science, Vol. 10, Issue 9
  • DOI: 10.1039/C7EE01232B

Defect-Assisted Photoinduced Halide Segregation in Mixed-Halide Perovskite Thin Films
journal, May 2017


Anomalous Optical Absorption Limit in InSb
journal, February 1954


Carrier lifetimes of >1 μs in Sn-Pb perovskites enable efficient all-perovskite tandem solar cells
journal, April 2019


Selecting tandem partners for silicon solar cells
journal, September 2016


Compositional Engineering for Efficient Wide Band Gap Perovskites with Improved Stability to Photoinduced Phase Segregation
journal, January 2018


Determination of Chloride Content in Planar CH 3 NH 3 PbI 3− x Cl x Solar Cells by Chemical Analysis
journal, August 2015

  • Cojocaru, Ludmila; Uchida, Satoshi; Jena, Ajay Kumar
  • Chemistry Letters, Vol. 44, Issue 8
  • DOI: 10.1246/cl.150385

Minimizing Current and Voltage Losses to Reach 25% Efficient Monolithic Two-Terminal Perovskite–Silicon Tandem Solar Cells
journal, August 2018


MAPbI3-xClx Mixed Halide Perovskite for Hybrid Solar Cells: The Role of Chloride as Dopant on the Transport and Structural Properties
journal, November 2013

  • Colella, Silvia; Mosconi, Edoardo; Fedeli, Paolo
  • Chemistry of Materials, Vol. 25, Issue 22, p. 4613-4618
  • DOI: 10.1021/cm402919x

Visualization and suppression of interfacial recombination for high-efficiency large-area pin perovskite solar cells
journal, July 2018

  • Stolterfoht, Martin; Wolff, Christian M.; Márquez, José A.
  • Nature Energy, Vol. 3, Issue 10
  • DOI: 10.1038/s41560-018-0219-8

Impact of Surfaces on Photoinduced Halide Segregation in Mixed-Halide Perovskites
journal, October 2018


Record Open‐Circuit Voltage Wide‐Bandgap Perovskite Solar Cells Utilizing 2D/3D Perovskite Heterostructure
journal, April 2019

  • Gharibzadeh, Saba; Abdollahi Nejand, Bahram; Jakoby, Marius
  • Advanced Energy Materials, Vol. 9, Issue 21
  • DOI: 10.1002/aenm.201803699

Mechanically-stacked perovskite/CIGS tandem solar cells with efficiency of 23.9% and reduced oxygen sensitivity
journal, January 2018

  • Shen, Heping; Duong, The; Peng, Jun
  • Energy & Environmental Science, Vol. 11, Issue 2
  • DOI: 10.1039/C7EE02627G

Anomalous Band Gap Behavior in Mixed Sn and Pb Perovskites Enables Broadening of Absorption Spectrum in Solar Cells
journal, May 2014

  • Hao, Feng; Stoumpos, Constantinos C.; Chang, Robert P. H.
  • Journal of the American Chemical Society, Vol. 136, Issue 22
  • DOI: 10.1021/ja5033259

Abnormal crystal growth in CH 3 NH 3 PbI 3−x Cl x using a multi-cycle solution coating process
journal, January 2015

  • Dong, Qingfeng; Yuan, Yongbo; Shao, Yuchuan
  • Energy & Environmental Science, Vol. 8, Issue 8
  • DOI: 10.1039/C5EE01179E

Effects of CsBr addition on the performance of CH3NH3PbI3-xClx-based solar cells
conference, January 2018

  • Ueoka, Naoki; Oku, Takeo; Ohishi, Yuya
  • THE IRAGO CONFERENCE 2017: A 360-degree Outlook on Critical Scientific and Technological Challenges for a Sustainable Society, AIP Conference Proceedings
  • DOI: 10.1063/1.5021939

Efficient Semitransparent Perovskite Solar Cells for 23.0%-Efficiency Perovskite/Silicon Four-Terminal Tandem Cells
journal, July 2016


Vertical recrystallization for highly efficient and stable formamidinium-based inverted-structure perovskite solar cells
journal, January 2017

  • Xie, Fengxian; Chen, Chun-Chao; Wu, Yongzhen
  • Energy & Environmental Science, Vol. 10, Issue 9
  • DOI: 10.1039/C7EE01675A

Solar cell efficiency tables (version 54)
journal, June 2019

  • Green, Martin A.; Dunlop, Ewan D.; Levi, Dean H.
  • Progress in Photovoltaics: Research and Applications, Vol. 27, Issue 7
  • DOI: 10.1002/pip.3171

Efficient Indium-Doped TiO x Electron Transport Layers for High-Performance Perovskite Solar Cells and Perovskite-Silicon Tandems
journal, November 2016

  • Peng, Jun; Duong, The; Zhou, Xianzhong
  • Advanced Energy Materials, Vol. 7, Issue 4
  • DOI: 10.1002/aenm.201601768

Transforming Hybrid Organic Inorganic Perovskites by Rapid Halide Exchange
journal, March 2015


Silicon heterojunction solar cell with interdigitated back contacts for a photoconversion efficiency over 26%
journal, March 2017


Infrared Light Management Using a Nanocrystalline Silicon Oxide Interlayer in Monolithic Perovskite/Silicon Heterojunction Tandem Solar Cells with Efficiency above 25%
journal, February 2019

  • Mazzarella, Luana; Lin, Yen‐Hung; Kirner, Simon
  • Advanced Energy Materials, Vol. 9, Issue 14
  • DOI: 10.1002/aenm.201803241

Reversible Halide Exchange Reaction of Organometal Trihalide Perovskite Colloidal Nanocrystals for Full-Range Band Gap Tuning
journal, July 2015


Grain Engineering for Perovskite/Silicon Monolithic Tandem Solar Cells with Efficiency of 25.4%
journal, January 2019


Bimolecular Additives Improve Wide-Band-Gap Perovskites for Efficient Tandem Solar Cells with CIGS
journal, July 2019


Mitigating Measurement Artifacts in TOF-SIMS Analysis of Perovskite Solar Cells
journal, August 2019

  • Harvey, Steven P.; Zhang, Fei; Palmstrom, Axel
  • ACS Applied Materials & Interfaces, Vol. 11, Issue 34
  • DOI: 10.1021/acsami.9b09445

Light Management: A Key Concept in High-Efficiency Perovskite/Silicon Tandem Photovoltaics
journal, May 2019

  • Jacobs, Daniel A.; Langenhorst, Malte; Sahli, Florent
  • The Journal of Physical Chemistry Letters, Vol. 10, Issue 11
  • DOI: 10.1021/acs.jpclett.8b03721

High Chloride Doping Levels Stabilize the Perovskite Phase of Cesium Lead Iodide
journal, May 2016


Effects of CuBr addition to CH3NH3PbI3(Cl) perovskite photovoltaic devices
conference, January 2018

  • Oku, Takeo; Ohishi, Yuya; Tanaka, Hiroki
  • THE IRAGO CONFERENCE 2017: A 360-degree Outlook on Critical Scientific and Technological Challenges for a Sustainable Society, AIP Conference Proceedings
  • DOI: 10.1063/1.5021923

CH 3 NH 3 PbCl 3 Single Crystals: Inverse Temperature Crystallization and Visible-Blind UV-Photodetector
journal, September 2015

  • Maculan, Giacomo; Sheikh, Arif D.; Abdelhady, Ahmed L.
  • The Journal of Physical Chemistry Letters, Vol. 6, Issue 19
  • DOI: 10.1021/acs.jpclett.5b01666

Tin–lead halide perovskites with improved thermal and air stability for efficient all-perovskite tandem solar cells
journal, January 2018

  • Leijtens, Tomas; Prasanna, Rohit; Bush, Kevin A.
  • Sustainable Energy & Fuels, Vol. 2, Issue 11
  • DOI: 10.1039/C8SE00314A

Understanding Degradation Mechanisms and Improving Stability of Perovskite Photovoltaics
journal, November 2018


Enabling Flexible All-Perovskite Tandem Solar Cells
journal, September 2019


Halide-Substituted Electronic Properties of Organometal Halide Perovskite Films: Direct and Inverse Photoemission Studies
journal, April 2016

  • Li, Chi; Wei, Jian; Sato, Mikio
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 18
  • DOI: 10.1021/acsami.6b02692

Ternary Halide Perovskites for Highly Efficient Solution-Processed Hybrid Solar Cells
journal, September 2016


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

Cesium Lead Halide Perovskites with Improved Stability for Tandem Solar Cells
journal, February 2016

  • Beal, Rachel E.; Slotcavage, Daniel J.; Leijtens, Tomas
  • The Journal of Physical Chemistry Letters, Vol. 7, Issue 5
  • DOI: 10.1021/acs.jpclett.6b00002

Probing Perovskite Inhomogeneity beyond the Surface: TOF-SIMS Analysis of Halide Perovskite Photovoltaic Devices
journal, July 2018

  • Harvey, Steven P.; Li, Zhen; Christians, Jeffrey A.
  • ACS Applied Materials & Interfaces, Vol. 10, Issue 34
  • DOI: 10.1021/acsami.8b07937

Roadmap and roadblocks for the band gap tunability of metal halide perovskites
journal, January 2017

  • Unger, E. L.; Kegelmann, L.; Suchan, K.
  • Journal of Materials Chemistry A, Vol. 5, Issue 23
  • DOI: 10.1039/C7TA00404D

Fully textured monolithic perovskite/silicon tandem solar cells with 25.2% power conversion efficiency
journal, June 2018


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


Chlorine in PbCl 2 -Derived Hybrid-Perovskite Solar Absorbers
journal, October 2015


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

A mixed-cation lead mixed-halide perovskite absorber for tandem solar cells
journal, January 2016


High-performance perovskite/Cu(In,Ga)Se 2 monolithic tandem solar cells
journal, August 2018


ABX3 Perovskites for Tandem Solar Cells
journal, December 2017


Hot carrier cooling mechanisms in halide perovskites
journal, November 2017


High-efficiency inverted semi-transparent planar perovskite solar cells in substrate configuration
journal, December 2016


Barrier Design to Prevent Metal-Induced Degradation and Improve Thermal Stability in Perovskite Solar Cells
journal, June 2018