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Cooling Mixed A-Site Halide Perovskites: Impact of Temperature on Optical and Structural Properties

Journal Article · · Chemistry of Materials
 [1];  [2];  [3];  [4];  [5];  [5];  [6];  [4];  [2];  [7]
  1. Rice Univ., Houston, TX (United States); Florida State Univ., Tallahassee, FL (United States)
  2. Florida State Univ., Tallahassee, FL (United States)
  3. Florida State Univ., Tallahassee, FL (United States). National High Magnetic Field Laboratory (MagLab)
  4. Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)
  5. Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  6. Univ. of Florida, Gainesville, FL (United States). National High Magnetic Field Laboratory (MagLab); Florida A & M University, Tallahassee, FL (United States); Florida State Univ., Tallahassee, FL (United States)
  7. Rice Univ., Houston, TX (United States)
The widespread utilization of perovskite-based photovoltaics requires probing both the structural and optical properties under extreme operating conditions to gain a holistic understanding of the material behavior under stressors. Here, in this study, we investigate the temperature-dependent behavior of mixed A-site cation lead triiodide perovskite thin films (85% methylammonium and 15% formamidinium) in the range from 300 to 20 K. Through a combination of optical and structural techniques, we find that the tetragonal-to-orthorhombic phase transition occurs at similar to 110 K for this perovskite composition, as indicated by the change in the diffraction pattern. With decreasing temperature, the quantum yield increases with a concurrent elongation of the carrier lifetimes, indicating suppression of nonradiative recombination pathways. Interestingly, in contrast to single A-site cation perovskites, an additional optical transition appears in the absorption spectrum when the phase transition is approached, which is also reflected in the emission spectrum. We propose that the splitting of the optical absorption and emission is due to local segregation of the mixed cation perovskite during the phase transition.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
Camille and Henry Dreyfus Foundation; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
2567002
Journal Information:
Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 19 Vol. 36; ISSN 1520-5002; ISSN 0897-4756
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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