skip to main content

DOE PAGESDOE PAGES

Title: Global Analysis of Perovskite Photophysics Reveals Importance of Geminate Pathways

Hybrid organic-inorganic perovskites demonstrate desirable photophysical behaviors and promising applications from efficient photovoltaics to lasing, but the fundamental nature of excited state species is still under debate. We also collected time-resolved photoluminescence of single-crystal nanoplates of methylammonium lead iodide perovskite (MAPbI3), with excitation over a range of fluences and repetition rates, to provide a more complete photophysical picture. A fundamentally different way of simulating the photophysics is developed that relies on unnormalized decays, global analysis over a large array of conditions, and inclusion of steady-state behavior; these details are critical to capturing observed behaviors. These additional constraints require inclusion of spatially-correlated pairs, along with free carriers and traps, demonstrating the importance of our comprehensive analysis. Modeling geminate and non-geminate pathways shows geminate processes are dominant at high carrier densities and early times. This combination of data and simulation provides a detailed picture of perovskite photophysics across multiple excitation regimes that was not previously available.
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ; ORCiD logo [1] ;  [1] ; ORCiD logo [1]
  1. Univ. of Wisconsin, Madison, WI (United States). Dept. of Chemistry
Publication Date:
Grant/Contract Number:
FG02-09ER46664; SC0002162
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 121; Journal Issue: 2; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Research Org:
Univ. of Wisconsin, Madison, WI (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Chicago Operations Office (CO)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1393446

Manger, Lydia H., Rowley, Matthew B., Fu, Yongping, Foote, Alexander K., Rea, Morgan T., Wood, Sharla L., Jin, Song, Wright, John C., and Goldsmith, Randall H.. Global Analysis of Perovskite Photophysics Reveals Importance of Geminate Pathways. United States: N. p., Web. doi:10.1021/acs.jpcc.6b11547.
Manger, Lydia H., Rowley, Matthew B., Fu, Yongping, Foote, Alexander K., Rea, Morgan T., Wood, Sharla L., Jin, Song, Wright, John C., & Goldsmith, Randall H.. Global Analysis of Perovskite Photophysics Reveals Importance of Geminate Pathways. United States. doi:10.1021/acs.jpcc.6b11547.
Manger, Lydia H., Rowley, Matthew B., Fu, Yongping, Foote, Alexander K., Rea, Morgan T., Wood, Sharla L., Jin, Song, Wright, John C., and Goldsmith, Randall H.. 2016. "Global Analysis of Perovskite Photophysics Reveals Importance of Geminate Pathways". United States. doi:10.1021/acs.jpcc.6b11547. https://www.osti.gov/servlets/purl/1393446.
@article{osti_1393446,
title = {Global Analysis of Perovskite Photophysics Reveals Importance of Geminate Pathways},
author = {Manger, Lydia H. and Rowley, Matthew B. and Fu, Yongping and Foote, Alexander K. and Rea, Morgan T. and Wood, Sharla L. and Jin, Song and Wright, John C. and Goldsmith, Randall H.},
abstractNote = {Hybrid organic-inorganic perovskites demonstrate desirable photophysical behaviors and promising applications from efficient photovoltaics to lasing, but the fundamental nature of excited state species is still under debate. We also collected time-resolved photoluminescence of single-crystal nanoplates of methylammonium lead iodide perovskite (MAPbI3), with excitation over a range of fluences and repetition rates, to provide a more complete photophysical picture. A fundamentally different way of simulating the photophysics is developed that relies on unnormalized decays, global analysis over a large array of conditions, and inclusion of steady-state behavior; these details are critical to capturing observed behaviors. These additional constraints require inclusion of spatially-correlated pairs, along with free carriers and traps, demonstrating the importance of our comprehensive analysis. Modeling geminate and non-geminate pathways shows geminate processes are dominant at high carrier densities and early times. This combination of data and simulation provides a detailed picture of perovskite photophysics across multiple excitation regimes that was not previously available.},
doi = {10.1021/acs.jpcc.6b11547},
journal = {Journal of Physical Chemistry. C},
number = 2,
volume = 121,
place = {United States},
year = {2016},
month = {12}
}