skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Highly Efficient Perovskite-Perovskite Tandem Solar Cells Reaching 80% of the Theoretical Limit in Photovoltage

Abstract

Organic–inorganic hybrid perovskite multijunction solar cells have immense potential to realize power conversion efficiencies (PCEs) beyond the Shockley–Queisser limit of single-junction solar cells; however, they are limited by large nonideal photovoltage loss (V oc,loss) in small- and large-bandgap subcells. Here, an integrated approach is utilized to improve the V oc of subcells with optimized bandgaps and fabricate perovskite–perovskite tandem solar cells with small V oc,loss. A fullerene variant, Indene-C 60 bis-adduct, is used to achieve optimized interfacial contact in a small-bandgap (≈1.2 eV) subcell, which facilitates higher quasi-Fermi level splitting, reduces nonradiative recombination, alleviates hysteresis instabilities, and improves V oc to 0.84 V. Compositional engineering of large-bandgap (≈1.8 eV) perovskite is employed to realize a subcell with a transparent top electrode and photostabilized V oc of 1.22 V. The resultant monolithic perovskite–perovskite tandem solar cell shows a high V oc of 1.98 V (approaching 80% of the theoretical limit) and a stabilized PCE of 18.5%. The significantly minimized nonideal V oc,loss is better than state-of-the-art silicon–perovskite tandem solar cells, which highlights the prospects of using perovskite–perovskite tandems for solar-energy generation. It also unlocks opportunities for solar water splitting using hybrid perovskites with solar-to-hydrogen efficiencies beyond 15%.

Authors:
 [1];  [1];  [1];  [2];  [1];  [2];  [3]
  1. Univ. of Washington, Seattle, WA (United States). Dept. of Materials Science and Engineering
  2. Univ. of Washington, Seattle, WA (United States). Dept. of Chemical Engineering. Molecular Engineering and Sciences Inst.
  3. Univ. of Washington, Seattle, WA (United States). Dept. of Materials Science and Engineering; City Univ. of Hong Kong (Hong Kong). Dept. of Biology and Chemistry
Publication Date:
Research Org.:
Univ. of Washington, Seattle, WA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office; National Science Foundation (NSF); Office of Naval Research (ONR) (United States); Asian Office of Aerospace Research and Development (AOARD) (United States)
OSTI Identifier:
1533046
Alternate Identifier(s):
OSTI ID: 1380026
Grant/Contract Number:  
EE0006710; DMR-1608279; ECC-1542101; N00014-17-1-2260; FA2386-15-1-4106
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 29; Journal Issue: 34; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; hysteresis and photostability; monolithic tandem; open-circuit voltage; optical simulations; solar water splitting

Citation Formats

Rajagopal, Adharsh, Yang, Zhibin, Jo, Sae Byeok, Braly, Ian L., Liang, Po-Wei, Hillhouse, Hugh W., and Jen, Alex K. -Y. Highly Efficient Perovskite-Perovskite Tandem Solar Cells Reaching 80% of the Theoretical Limit in Photovoltage. United States: N. p., 2017. Web. doi:10.1002/adma.201702140.
Rajagopal, Adharsh, Yang, Zhibin, Jo, Sae Byeok, Braly, Ian L., Liang, Po-Wei, Hillhouse, Hugh W., & Jen, Alex K. -Y. Highly Efficient Perovskite-Perovskite Tandem Solar Cells Reaching 80% of the Theoretical Limit in Photovoltage. United States. https://doi.org/10.1002/adma.201702140
Rajagopal, Adharsh, Yang, Zhibin, Jo, Sae Byeok, Braly, Ian L., Liang, Po-Wei, Hillhouse, Hugh W., and Jen, Alex K. -Y. Mon . "Highly Efficient Perovskite-Perovskite Tandem Solar Cells Reaching 80% of the Theoretical Limit in Photovoltage". United States. https://doi.org/10.1002/adma.201702140. https://www.osti.gov/servlets/purl/1533046.
@article{osti_1533046,
title = {Highly Efficient Perovskite-Perovskite Tandem Solar Cells Reaching 80% of the Theoretical Limit in Photovoltage},
author = {Rajagopal, Adharsh and Yang, Zhibin and Jo, Sae Byeok and Braly, Ian L. and Liang, Po-Wei and Hillhouse, Hugh W. and Jen, Alex K. -Y.},
abstractNote = {Organic–inorganic hybrid perovskite multijunction solar cells have immense potential to realize power conversion efficiencies (PCEs) beyond the Shockley–Queisser limit of single-junction solar cells; however, they are limited by large nonideal photovoltage loss (V oc,loss) in small- and large-bandgap subcells. Here, an integrated approach is utilized to improve the V oc of subcells with optimized bandgaps and fabricate perovskite–perovskite tandem solar cells with small V oc,loss. A fullerene variant, Indene-C60 bis-adduct, is used to achieve optimized interfacial contact in a small-bandgap (≈1.2 eV) subcell, which facilitates higher quasi-Fermi level splitting, reduces nonradiative recombination, alleviates hysteresis instabilities, and improves V oc to 0.84 V. Compositional engineering of large-bandgap (≈1.8 eV) perovskite is employed to realize a subcell with a transparent top electrode and photostabilized V oc of 1.22 V. The resultant monolithic perovskite–perovskite tandem solar cell shows a high V oc of 1.98 V (approaching 80% of the theoretical limit) and a stabilized PCE of 18.5%. The significantly minimized nonideal V oc,loss is better than state-of-the-art silicon–perovskite tandem solar cells, which highlights the prospects of using perovskite–perovskite tandems for solar-energy generation. It also unlocks opportunities for solar water splitting using hybrid perovskites with solar-to-hydrogen efficiencies beyond 15%.},
doi = {10.1002/adma.201702140},
url = {https://www.osti.gov/biblio/1533046}, journal = {Advanced Materials},
issn = {0935-9648},
number = 34,
volume = 29,
place = {United States},
year = {2017},
month = {7}
}

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

Citation Metrics:
Cited by: 38 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

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


Hybrid organic—inorganic perovskites: low-cost semiconductors with intriguing charge-transport properties
journal, January 2016


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


Metal halide perovskites for energy applications
journal, May 2016


High Efficiency Tandem Thin-Perovskite/Polymer Solar Cells with a Graded Recombination Layer
journal, March 2016


Organic–Inorganic Perovskites: Structural Versatility for Functional Materials Design
journal, March 2016


The rapid evolution of highly efficient perovskite solar cells
journal, January 2017


Modeling Anomalous Hysteresis in Perovskite Solar Cells
journal, September 2015


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


Open Circuit Potential Build-Up in Perovskite Solar Cells from Dark Conditions to 1 Sun
journal, October 2015


Spectral Features and Charge Dynamics of Lead Halide Perovskites: Origins and Interpretations
journal, January 2016


High Open-Circuit Voltages in Tin-Rich Low-Bandgap Perovskite-Based Planar Heterojunction Photovoltaics
journal, November 2016


Solar cell efficiency tables (version 49): Solar cell efficiency tables (version 49)
journal, November 2016


Light-Induced Phase Segregation in Halide-Perovskite Absorbers
journal, November 2016


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


Lead-free organic–inorganic tin halide perovskites for photovoltaic applications
journal, January 2014


Stable Low-Bandgap Pb-Sn Binary Perovskites for Tandem Solar Cells
journal, August 2016


Roles of Fullerene-Based Interlayers in Enhancing the Performance of Organometal Perovskite Thin-Film Solar Cells
journal, February 2015


Inverted Current-Voltage Hysteresis in Mixed Perovskite Solar Cells: Polarization, Energy Barriers, and Defect Recombination
journal, July 2016


Photovoltaic materials: Present efficiencies and future challenges
journal, April 2016


Water photolysis at 12.3% efficiency via perovskite photovoltaics and Earth-abundant catalysts
journal, September 2014


Defect states in perovskite solar cells associated with hysteresis and performance
journal, October 2016


Carrier Diffusion Lengths of over 500 nm in Lead-Free Perovskite CH 3 NH 3 SnI 3 Films
journal, October 2016


A two-terminal perovskite/perovskite tandem solar cell
journal, January 2016


Monolithic Perovskite-CIGS Tandem Solar Cells via In Situ Band Gap Engineering
journal, September 2015


Solvent-Mediated Crystallization of CH3NH3SnI3 Films for Heterojunction Depleted Perovskite Solar Cells
journal, August 2015


Quantifying Losses in Open-Circuit Voltage in Solution-Processable Solar Cells
journal, July 2015


Stabilized Wide Bandgap MAPbBr x I 3- x Perovskite by Enhanced Grain Size and Improved Crystallinity
journal, December 2015


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


Long-Range Balanced Electron- and Hole-Transport Lengths in Organic-Inorganic CH3NH3PbI3
journal, October 2013


Effect of Structural Phase Transition on Charge-Carrier Lifetimes and Defects in CH 3 NH 3 SnI 3 Perovskite
journal, March 2016


Fabrication of Efficient Low-Bandgap Perovskite Solar Cells by Combining Formamidinium Tin Iodide with Methylammonium Lead Iodide
journal, September 2016


Efficient Monolithic Perovskite/Perovskite Tandem Solar Cells
journal, December 2016


50% Sn-Based Planar Perovskite Solar Cell with Power Conversion Efficiency up to 13.6%
journal, August 2016


Stabilized Wide Bandgap Perovskite Solar Cells by Tin Substitution
journal, November 2016


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


Perovskite photonic sources
journal, April 2016


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


Monolithic perovskite/silicon-heterojunction tandem solar cells processed at low temperature
journal, January 2016


High-efficiency tandem perovskite solar cells
journal, August 2015


Perovskite-perovskite tandem photovoltaics with optimized band gaps
journal, October 2016


Chemically diverse and multifunctional hybrid organic–inorganic perovskites
journal, February 2017


Photoinduced Emissive Trap States in Lead Halide Perovskite Semiconductors
journal, September 2016


Efficient Monolithic Perovskite/Silicon Tandem Solar Cell with Cell Area >1 cm 2
journal, December 2015


High Open-Circuit Voltages in Tin-Rich Low-Bandgap Perovskite-Based Planar Heterojunction Photovoltaics
text, January 2017


    Works referencing / citing this record:

    Two‐Terminal Perovskites Tandem Solar Cells: Recent Advances and Perspectives
    journal, May 2019


    Reduced open-circuit voltage loss for highly efficient low-bandgap perovskite solar cells via suppression of silver diffusion
    journal, January 2019


    Interplay of Structural and Optoelectronic Properties in Formamidinium Mixed Tin-Lead Triiodide Perovskites
    journal, June 2018


    Low‐Bandgap Mixed Tin‐Lead Perovskites and Their Applications in All‐Perovskite Tandem Solar Cells
    journal, February 2019


    Ideal Bandgap Organic-Inorganic Hybrid Perovskite Solar Cells
    journal, November 2017


    Large-Grain Tin-Rich Perovskite Films for Efficient Solar Cells via Metal Alloying Technique
    journal, January 2018


    Toward Perovskite Solar Cell Commercialization: A Perspective and Research Roadmap Based on Interfacial Engineering
    journal, June 2018


    “Unleaded” Perovskites: Status Quo and Future Prospects of Tin‐Based Perovskite Solar Cells
    journal, September 2018


    Low‐Cost Counter‐Electrode Materials for Dye‐Sensitized and Perovskite Solar Cells
    journal, May 2019


    Low Work Function Surface Modifiers for Solution-Processed Electronics: A Review
    journal, April 2018


    Hybrid Perovskites: Prospects for Concentrator Solar Cells
    journal, February 2018


    Modeling Thin Film Solar Cells: From Organic to Perovskite
    journal, November 2019


    Reverse Bias Behavior of Halide Perovskite Solar Cells
    journal, December 2017


    Solution-Processed Low-Bandgap CuIn(S,Se) 2 Absorbers for High-Efficiency Single-Junction and Monolithic Chalcopyrite-Perovskite Tandem Solar Cells
    journal, August 2018


    Inorganic Materials as Hole Selective Contacts and Intermediate Tunnel Junction Layer for Monolithic Perovskite-CIGSe Tandem Solar Cells
    journal, September 2018


    Improved Efficiency and Stability of Pb/Sn Binary Perovskite Solar Cells Fabricated by Galvanic Displacement Reaction
    journal, January 2019


    Reducing Saturation-Current Density to Realize High-Efficiency Low-Bandgap Mixed Tin-Lead Halide Perovskite Solar Cells
    journal, November 2018


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


    Wide‐Bandgap Perovskite/Gallium Arsenide Tandem Solar Cells
    journal, December 2019


    Trap States, Electric Fields, and Phase Segregation in Mixed‐Halide Perovskite Photovoltaic Devices
    journal, January 2020


    GaAs/silicon PVMirror tandem photovoltaic mini‐module with 29.6% efficiency with respect to the outdoor global irradiance
    journal, January 2019


    Optical Design in Perovskite Solar Cells
    journal, April 2019


    Crystallization, Properties, and Challenges of Low-Bandgap Sn-Pb Binary Perovskites
    journal, July 2018


    Energy Level Tuning of PEDOT:PSS for High Performance Tin-Lead Mixed Perovskite Solar Cells
    journal, November 2018


    Strain engineering in perovskite solar cells and its impacts on carrier dynamics
    journal, February 2019


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


    High voltage vacuum-deposited CH 3 NH 3 PbI 3 –CH 3 NH 3 PbI 3 tandem solar cells
    journal, January 2018


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


    Revealing the origin of voltage loss in mixed-halide perovskite solar cells
    journal, January 2020


    On understanding bandgap bowing and optoelectronic quality in Pb–Sn alloy hybrid perovskites
    journal, January 2019


    Tin( iv ) dopant removal through anti-solvent engineering enabling tin based perovskite solar cells with high charge carrier mobilities
    journal, January 2019


    Thin‐film solar cells exceeding 22% solar cell efficiency: An overview on CdTe-, Cu(In,Ga)Se 2 -, and perovskite-based materials
    journal, December 2018


    Wide-bandgap, low-bandgap, and tandem perovskite solar cells
    journal, July 2019


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