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

Title: Overcoming the Photovoltage Plateau in Large Bandgap Perovskite Photovoltaics

Abstract

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 overcomemore » 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.« less

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [2]
  1. Univ. of Washington, Seattle, WA (United States)
  2. Univ. of Washington, Seattle, WA (United States); City Univ. of Hong Kong (China)
Publication Date:
Research Org.:
Univ. of Washington, Seattle, WA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Solar Energy Technologies Office (EE-4S)
OSTI Identifier:
1436489
Grant/Contract Number:  
[EE0006710]
Resource Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
[ Journal Volume: 18; Journal Issue: 6]; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; Tandem solar cell; optoelectronic quality; 2D−3D perovskite; charge recombination dynamics; mixed-halide phase segregation; open-circuit voltage bottleneck

Citation Formats

Rajagopal, Adharsh, Stoddard, Ryan J., Jo, Sae Byeok, Hillhouse, Hugh W., and Jen, Alex K. -Y. Overcoming the Photovoltage Plateau in Large Bandgap Perovskite Photovoltaics. United States: N. p., 2018. Web. doi:10.1021/acs.nanolett.8b01480.
Rajagopal, Adharsh, Stoddard, Ryan J., Jo, Sae Byeok, Hillhouse, Hugh W., & Jen, Alex K. -Y. Overcoming the Photovoltage Plateau in Large Bandgap Perovskite Photovoltaics. United States. doi:10.1021/acs.nanolett.8b01480.
Rajagopal, Adharsh, Stoddard, Ryan J., Jo, Sae Byeok, Hillhouse, Hugh W., and Jen, Alex K. -Y. Mon . "Overcoming the Photovoltage Plateau in Large Bandgap Perovskite Photovoltaics". United States. doi:10.1021/acs.nanolett.8b01480. https://www.osti.gov/servlets/purl/1436489.
@article{osti_1436489,
title = {Overcoming the Photovoltage Plateau in Large Bandgap Perovskite Photovoltaics},
author = {Rajagopal, Adharsh and Stoddard, Ryan J. and Jo, Sae Byeok and Hillhouse, Hugh W. and Jen, Alex K. -Y.},
abstractNote = {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.},
doi = {10.1021/acs.nanolett.8b01480},
journal = {Nano Letters},
number = [6],
volume = [18],
place = {United States},
year = {2018},
month = {5}
}

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

Citation Metrics:
Cited by: 10 works
Citation information provided by
Web of Science

Figures / Tables:

Figure 1 Figure 1: Comparison of the figure-of-merit (open-circuit voltage, Voc) for mixed-halide hybrid PVKSCs reported in literature in perspective to this work. (a) Voc and (b) corresponding Voc/Voc,SQ as a function of bandgap (Eg) for works in the 1.6−1.9 eV Eg range. Red stars correspond to values obtained in this work.more » Citations for points 1−22 and an associated discussion are provided in Supporting Information.« less

Save / Share:

Works referencing / citing this record:

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


Heterogeneity at multiple length scales in halide perovskite semiconductors
journal, July 2019

  • Tennyson, Elizabeth M.; Doherty, Tiarnan A. S.; Stranks, Samuel D.
  • Nature Reviews Materials, Vol. 4, Issue 9
  • DOI: 10.1038/s41578-019-0125-0

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