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

Title: Overcoming the Photovoltage Plateau in Large Bandgap Perovskite Photovoltaics

Journal Article · · Nano Letters

Development of large bandgap (1.80-1.85 eV Eg) perovskite is crucial for perovskite-perovskite tandem solar cells. However, the performance of 1.80-1.85 eV Eg perovskite solar cells (PVKSCs) are significantly lagging their counterparts in the 1.60-1.75 eV Eg range. This is because the photovoltage (Voc) does not proportionally increase with Eg due to lower optoelectronic quality of conventional (MA,FA,Cs)Pb(I,Br)3 and results in a photovoltage plateau (Voc limited to 80% of the theoretical limit for ~1.8 eV Eg). Here, we incorporate phenyl- ethylammonium (PEA) in a mixed-halide perovskite composition to solve the inherent material-level challenges in 1.80-1.85 eV Eg perovskites. The amount of PEA incorporation governs the topography and optoelectronic properties of resultant films. Detailed structural and spectroscopic characterization reveal the characteristic trends in crystalline size, orientation, and charge carrier recombination dynamics and rationalize the origin of improved material quality with higher luminescence. With careful interface optimization, the improved material characteristics were translated to devices and Voc values of 1.30-1.35 V were achieved, which correspond to 85-87% of the theoretical limit. Using an optimal amount of PEA incorporation to balance the increase in Voc and the decrease in charge collection, a highest power conversion efficiency of 12.2% was realized. Our results clearly overcome the photovoltage plateau in the 1.80-1.85 eV Eg range and represent the highest Voc achieved for mixed-halide PVKSCs. This study provides widely translatable insights, an important breakthrough, and a promising platform for next- generation perovskite tandems.

Research Organization:
Univ. of Washington, Seattle, WA (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office
Grant/Contract Number:
EE0006710
OSTI ID:
1436489
Journal Information:
Nano Letters, Vol. 18, Issue 6; ISSN 1530-6984
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 77 works
Citation information provided by
Web of Science

References (55)

Understanding the physical properties of hybrid perovskites for photovoltaic applications journal July 2017
Intriguing Optoelectronic Properties of Metal Halide Perovskites journal June 2016
Organic–Inorganic Perovskites: Structural Versatility for Functional Materials Design journal March 2016
Photovoltaic materials: Present efficiencies and future challenges journal April 2016
Solar cell efficiency tables (version 51)
  • Green, Martin A.; Hishikawa, Yoshihiro; Dunlop, Ewan D.
  • Progress in Photovoltaics: Research and Applications, Vol. 26, Issue 1 https://doi.org/10.1002/pip.2978
journal December 2017
Toward Perovskite Solar Cell Commercialization: A Perspective and Research Roadmap Based on Interfacial Engineering journal June 2018
Promises and challenges of perovskite solar cells journal November 2017
Capturing the Sun: A Review of the Challenges and Perspectives of Perovskite Solar Cells journal June 2017
ABX3 Perovskites for Tandem Solar Cells journal December 2017
Metal halide perovskite tandem and multiple-junction photovoltaics journal November 2017
Environmental analysis of perovskites and other relevant solar cell technologies in a tandem configuration journal January 2017
Perovskite-perovskite tandem photovoltaics with optimized band gaps journal October 2016
Highly Efficient Perovskite-Perovskite Tandem Solar Cells Reaching 80% of the Theoretical Limit in Photovoltage journal July 2017
23.6%-efficient monolithic perovskite/silicon tandem solar cells with improved stability journal February 2017
Roadmap and roadblocks for the band gap tunability of metal halide perovskites journal January 2017
Iodide management in formamidinium-lead-halide–based perovskite layers for efficient solar cells journal June 2017
Maximizing and stabilizing luminescence from halide perovskites with potassium passivation journal March 2018
Light-Induced Anion Phase Segregation in Mixed Halide Perovskites journal November 2017
Current-Induced Phase Segregation in Mixed Halide Hybrid Perovskites and its Impact on Two-Terminal Tandem Solar Cell Design journal July 2017
Optoelectronic Quality and Stability of Hybrid Perovskites from MAPbI 3 to MAPbI 2 Br Using Composition Spread Libraries journal January 2016
Correlation between Photoluminescence and Carrier Transport and a Simple In Situ Passivation Method for High-Bandgap Hybrid Perovskites journal July 2017
Rationalizing the light-induced phase separation of mixed halide organic–inorganic perovskites journal August 2017
Band Tailing and Deep Defect States in CH 3 NH 3 Pb(I 1– x Br x ) 3 Perovskites As Revealed by Sub-Bandgap Photocurrent journal February 2017
Stabilized Wide Bandgap Perovskite Solar Cells by Tin Substitution journal November 2016
A mixed-cation lead mixed-halide perovskite absorber for tandem solar cells journal January 2016
Matching Charge Extraction Contact for Wide-Bandgap Perovskite Solar Cells journal May 2017
Rubidium Multication Perovskite with Optimized Bandgap for Perovskite-Silicon Tandem with over 26% Efficiency journal April 2017
Synergistic Effects of Lead Thiocyanate Additive and Solvent Annealing on the Performance of Wide-Bandgap Perovskite Solar Cells journal April 2017
Amide‐Catalyzed Phase‐Selective Crystallization Reduces Defect Density in Wide‐Bandgap Perovskites journal February 2018
Defect passivation in hybrid perovskite solar cells using quaternary ammonium halide anions and cations journal June 2017
Benzylamine-Treated Wide-Bandgap Perovskite with High Thermal-Photostability and Photovoltaic Performance journal September 2017
Efficient ambient-air-stable solar cells with 2D–3D heterostructured butylammonium-caesium-formamidinium lead halide perovskites journal August 2017
Mixed-Halide Perovskites with Stabilized Bandgaps journal October 2017
Incorporation of rubidium cations into perovskite solar cells improves photovoltaic performance journal September 2016
Defect Passivation via a Graded Fullerene Heterojunction in Low-Bandgap Pb–Sn Binary Perovskite Photovoltaics journal October 2017
Ligand-Stabilized Reduced-Dimensionality Perovskites journal February 2016
Ultralow Self-Doping in Two-dimensional Hybrid Perovskite Single Crystals journal June 2017
Passivation of Grain Boundaries by Phenethylammonium in Formamidinium-Methylammonium Lead Halide Perovskite Solar Cells journal February 2018
Dimensional Engineering of a Graded 3D-2D Halide Perovskite Interface Enables Ultrahigh V oc Enhanced Stability in the p-i-n Photovoltaics journal July 2017
Stabilization of the Metastable Lead Iodide Perovskite Phase via Surface Functionalization journal June 2017
Mixed Cation FA x PEA 1- x PbI 3 with Enhanced Phase and Ambient Stability toward High-Performance Perovskite Solar Cells journal September 2016
Perovskite energy funnels for efficient light-emitting diodes journal June 2016
Charge-Carrier Dynamics in 2D Hybrid Metal–Halide Perovskites journal October 2016
Optical Properties and Modeling of 2D Perovskite Solar Cells journal July 2017
Composite Nature of Layered Hybrid Perovskites: Assessment on Quantum and Dielectric Confinements and Band Alignment journal February 2018
Hybrid perovskite films approaching the radiative limit with over 90% photoluminescence quantum efficiency journal April 2018
Local Observation of Phase Segregation in Mixed-Halide Perovskite journal February 2018
Carrier Diffusion Lengths of over 500 nm in Lead-Free Perovskite CH 3 NH 3 SnI 3 Films journal October 2016
Spatially segregated free-carrier and exciton populations in individual lead halide perovskite grains journal March 2017
Band filling with free charge carriers in organometal halide perovskites journal August 2014
Hybrid Perovskites for Photovoltaics: Charge-Carrier Recombination, Diffusion, and Radiative Efficiencies journal December 2015
Grain-Size-Limited Mobility in Methylammonium Lead Iodide Perovskite Thin Films journal August 2016
Facet-dependent photovoltaic efficiency variations in single grains of hybrid halide perovskite journal July 2016
Ideal Bandgap Organic-Inorganic Hybrid Perovskite Solar Cells journal November 2017
Compositional Engineering for Efficient Wide Band Gap Perovskites with Improved Stability to Photoinduced Phase Segregation journal January 2018

Cited By (20)

Monolithic all-perovskite tandem solar cells with 24.8% efficiency exploiting comproportionation to suppress Sn(ii) oxidation in precursor ink journal September 2019
Two‐Terminal Perovskites Tandem Solar Cells: Recent Advances and Perspectives journal May 2019
Divalent hard Lewis acid doped CsPbBr 3 films for 9.63%-efficiency and ultra-stable all-inorganic perovskite solar cells journal January 2019
Record Open‐Circuit Voltage Wide‐Bandgap Perovskite Solar Cells Utilizing 2D/3D Perovskite Heterostructure journal April 2019
Self‐Powered Sensors Enabled by Wide‐Bandgap Perovskite Indoor Photovoltaic Cells journal August 2019
Lanthanide Ions Doped CsPbBr 3 Halides for HTM-Free 10.14%-Efficiency Inorganic Perovskite Solar Cell with an Ultrahigh Open-Circuit Voltage of 1.594 V journal September 2018
Wide‐Bandgap Perovskite/Gallium Arsenide Tandem Solar Cells journal December 2019
Stabilizing halide perovskite surfaces for solar cell operation with wide-bandgap lead oxysalts journal August 2019
Understanding macroscale functionality of metal halide perovskites in terms of nanoscale heterogeneities journal December 2018
Wide-bandgap, low-bandgap, and tandem perovskite solar cells journal July 2019
Correlating hysteresis phenomena with interfacial charge accumulation in perovskite solar cells journal January 2020
Tailoring the Functionality of Organic Spacer Cations for Efficient and Stable Quasi‐2D Perovskite Solar Cells journal April 2019
Nonradiative Recombination in Perovskite Solar Cells: The Role of Interfaces journal October 2019
On understanding bandgap bowing and optoelectronic quality in Pb–Sn alloy hybrid perovskites journal January 2019
Heterogeneity at multiple length scales in halide perovskite semiconductors journal July 2019
Boosting Photovoltaic Performance for Lead Halide Perovskites Solar Cells with BF 4 Anion Substitutions journal February 2019
Imperfections and their passivation in halide perovskite solar cells text January 2019
Heterogeneity at multiple length scales in halide perovskite semiconductors text January 2019
Stabilizing halide perovskite surfaces for solar cell operation with wide-bandgap lead oxysalts text January 2019
Nonradiative Recombination in Perovskite Solar Cells: The Role of Interfaces text January 2019

Figures / Tables (6)